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February  10,  1&12. 


U.  S.  DEPARTMENT  OP  AGRICULTURE, 

BUREAU  OF  CHEMISTRY— BULLETIN  No.  147. 


H.  W.  WILEY,  ciukk  of  Bureau. 


COAL-TAR  COLORS  USED  IN 
FOOD  PRODUCTS. 


BY 


BERXILYRD  C.  HESSE,   Ph.  D. 

Exp*  ___ 


m 


1    ^o«n 


U.S.  DEPOSITORY 


Issued  February  10,  1912. 

U.  S.  DEPARTMENT  OF  AGRICULTURE, 

BUREAU  OF  CHEMISTRY—  BULLETIN  No.  147. 

H.  \Y.  WILEY,  Chief  of  Bureau. 


COAL-TAR  COLORS  USED  IN 
FOOD  PRODUCTS. 


BY 


BERNHARD  C.  HESSE,  Ph.  D. 

Expert,  Bureau  Chemistry. 


w  \sinv. 
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18U. 


ORGANIZATION  OF  BUREAU  OF  CHEMISTRY. 

H.  TV.  Wiley,  Chemist  and  Chief  of  Bureau. 

F.  L.  Dunlap,  Associate  Chemist,  and  Acting  Chief  in  absence  of  Chief 

W.  D.  Bigelow,  Assistant  Chief  of  Bureau. 

F.  B.  Linton,  Chief  Clerk. 

A.  L.  Pierce,  Editor. 

A.  E.  Draper,  Librarian. 

Division  of  Foods,  W.  D.  Bigelow,  Chief. 

Food-Inspection  Laboratory,  L.  M.  Tolman,  Chief. 

Food  Technology  Laboratory,  E.  M.  Chace,  Chief  and  Assistant  Chief  of  Division. 

Oil,  Fat,  and  Wax  Laboratory,  H.  S.  Bailey,  Chief 
Division  of  Drugs,  L.  F.  Kebler,  Chief. 

Drug-Inspection  Laboratory,  G.  W.  Hoover,  Chief. 

Synthetic  Products  Laboratory,  W.  0.  Emery,  Chief. 

Essential  Oils  Laboratory,  under  Chief  of  Division. 

Pharmacological  Laboratory,  Wm.  Salant,  Chief. 
Chief  Food  and  Drug  Inspector,  W.  G.  Campbell. 
Miscellaneous  Division,  J.  K.  Haywood,  Chief. 

Water  Laboratory,  W.  W.  Skinner,  Chief. 

Cattle-Food  and  Grain  Laboratory,  G.  L.  Bidwell,  Acting. 

Insecticide  and  Fungicide  Laboratory,  C.  C.  McDonnell,  Chief. 

Trade  Wastes  Laboratory,  under  Chief  of  Division. 
Contracts  Laboratory,  P.  H.  Walker,  Chief. 
Dairy  Laboratory,  G.  E.  Patrick,  Chief. 
Food  Research  Laboratory,  M.  E.  Pennington,  Chief. 
Leather  and  Paper  Laboratory,  F.  P.  Veitch,  Chief. 
Micro  chemical  Laboratory,  B.J.  Howard,  Chief. 
Physical  Chemistry  Laboratory,  C.  S.  Hudson,  Chief. 
Sugar  Laboratory,  A.  H.  Bryan,  Chief. 
Sections: 

Animal  Physiological  Chemistry,  F.  C.  Weber,  in  Charge. 

Bacteriological  Chemistry,  G.  W.  Stiles,  in  Charge. 

Enological  Chemistry,  W.  B.  Alwood,  in  Charge. 

Nitrogen,  T.  C.  Trescot,  in  Charge. 

Plant  Physiological  Chemistry,  J.  A.  Le  Clerc,  Chief. 
Food  and  Drug  Inspection  Laboratories: 

Boston,  B.  II.  Smith,  Chief 

Buffalo,  W.  L.  Dubois,  Chief. 

Chicago,  A.  L.  Winton,  Chief. 

Cincinnati,  B.  R.  Hart,  Chief. 

Denver,  R.  S.  Hiltner,  Chief. 

Detroit,  II.  L.  ScnuLz,  Chief. 

Galveston,  T.  F.  Pappe,  Chief. 

Honolulu,  Hawaii, 

Kansas  City,  Mo.,  F.  W.  Liepsner,  Chirf. 
ille,  R.  W.  Bjj  i  "M.  ( 'hUf. 

New  Orleans,  W.  J.  McGee,  Chief. 

N*\v  York,  It.  E.  Doolittlk,  Chief. 

Omaha,  S.  H.  Ross,  Chief. 

Philadelphia,  C.  B.  Brinton,  Chief. 

Pittsburg,  M.  C,  Albrbch,  Chief. 

Portland,  <  hreg.,  A.  I..  Knisei  r,  Chief. 

si.  Louis,  D,  Bj  Bisbbi,  (  hief. 
Paul,  A.  s.  Mm  hi  1 1,  Chief. 
d  Francisco,  K.  A.  Gould,  (  hief. 

Ban  Juan,  Porto  Rico,  A.  E.  Taylor,  Acting 

iimah,  \Y.  I    .   Ill  hn  ii,  (  hitf. 

Seattle,  II.  M.  Loo  mis,  Chief. 
2 


LETTER  OF  TRANSMITTAL. 


U.  S.  Department  of  Agriculture, 

Bureau  of  Chemistry, 
'Washington,  D.  C,  January  31,  1911. 
Sir:  I  have  the  honor  to  transmit  for  your  approval  a  report  by 
Bernhard  C.  Hesse,  a  color  expert,  containing  both  original  chemical 
work  done  in  the  bureau  since  the  passage  of  the  food  law  on  anilin 
dyes  used  for  foods,  and  a  valuable  and  extensive  compilation  of  the 
lit  (Mature  of  the  subject,  especially  with  reference  to  the  harmfulness 
of  coal-tar  colors  and  their  physiological  effects.  These  data  formed 
the  basis  of  the  opinions  stated  in  Food  Inspection  Decisions  76,  77, 
and  106,  and  are  presented  in  detail  as  of  scientific  and  practical 
interest  to  all  those  concerned  in  the  use  of  coal-tar  colors  in  foods, 
whether  as  manufacturers,  food  officials,  or  consumers.  1  recommend 
the  publication  of  this  report  as  Bulletin  No.  147  of  the  Bureau  of 
Chemistry. 

Respect  fully,  II.  W.  Wiley,  Chief. 

Hon.  James  Wilson, 

Secretary  cf  Agriculture, 


CONTEXTS. 


Page. 

Introduction 9 

Purpose  of  the  investigation 9 

Number  of  colors  permitted 11 

Quality  and  efficiency  of  colors  permitted 12 

I.  Identity  of  coal-tar  colors  used  in  food  products  in  the  United  States 

in  1907 15 

Collection  of  samples 15 

Classification  of  samples  submitted 17 

Green  Table  numbers 17 

Source 18 

Patents 18 

Shades  of  color 19 

II.  Purposes  of  food  coloring 23 

HI.  Food  color  requirements 25 

Adaptability  for  special  purposes 25 

Proportion  of  coal-tar  color  used 26 

Suitability  of  shades  of  permitted  colors  and  mixtures  of  panic 28 

IV.  Conformity   of  food    color   market,   1907,    to  recommendations  of  the 

National  Confectioners'  Association,  1899 30 

V.  Some  legal  enactments  relative  to  the  use  of  coal-tar  dyes 35 

List  of  thirteen  foreign  legal  enactments 35 

Summary  of  colors  permitted  by  .these  legal  enactments 35 

Colors  said  to  be  permitted  under  the  German  law  of  1887 37 

Definitenese  and  detail  necessary  to  effect  quality  control 40 

State  laws  prohibiting  the  use  of  colors  in  certain  foods,  1909 41 

VI.  Recommendations  by  associations  and  individuals  as  to  use  of  coal-tar 

dyes  as  food  colors 42 

Oazeneuve  and  Lupine 12 

Society  of  Swiss  Analytical  < ihemista id 

Tschireh 43 

Eayser 44 

\W\  l it 

National  Confectioners'  Association 45 

Bchacherl 45 

Classification  of  recommendations  in  the  literal ure 46 

Conclusions 47 

VII.  Recommendations  made  by  United  States  color  industries  and  trades 

to  the  Department  of  Agriculture 17 

Antagonistic  to  all  added  artificial  color 

Concerning  restrictions  and  requirements 48 

Vm.  Investigations,  other  than  on  animals,  bearing  on  the  harmfulness  of 

coal-tar  colors 

l'l-'fter ;,1 

Winogradow 

Eeidenhain 

Other  authors M 


6  CONSENTS. 

Page. 

IX.  Compilation  under  the  Green  Table  numbers  of  all  information  avail- 

able as  to  the  suitability  of  coal-tar  colors  for  food 56 

General  statements 56 

Classification  of  opinions  in  literature  and  in  legal  enactments  showing 

condition  of  the  market  in  1907 62 

Classification  according  to  chemical  composition  and  suitability 64 

Physiological  action  of  coal-tar  dyes 67 

Summary  of  symptoms 67 

Experiments  on  dogs 67 

Experiments  on  human  beings 70 

Experiments  on  small  animals 71 

General  statements 71 

Complete  detailed  statement  of  all  combined  data 74 

Abbreviations  of  authorities  cited 74 

Tabulation  by  Green  Table  numbers  of  physiological  and  other  data  75 

Alphabetical  index  of  trade  names  of  coal-tar  colors 148 

X.  Dosage  and  symptoms 153 

Confectioner's  list  as  a  basis  for  a  rule 153 

Lehmann's  rules 158 

Santori's  work  as  a  guide  to  a  rule 158 

Young's  rule 159 

XL  Oil-soluble  or  fat  colors 159 

XII.  Rules  and  reasons  for  selecting  the  seven  colors  permitted  by  F.  I.  D.  76. .  161 

Statement  of  rules 161 

Analysis  of  three  recommendations  made  to  the  Department  of  Agri- 
culture    162 

Process  of  elimination 166 

Reasons  for  adding  Ponceau  3R 167 

Quality,  cleanliness,  and  efficiency ' 169 

XHI.  Lists  of  colors  subsequently  recommended  by  individuals  and  asso- 
ciations    169 

Ernst 170 

M  uttelet's  interpretation  of  the  French  law 171 

Second  International  White  Cross  Congress 172 

Beythien  and  Ilempel 173 

Summary  of  three  preceding  recommendations 174 

Unpublished  recommendations  of  a  manufacturer 177 

Belial 177 

Conclusions 178 

XIV    Chemical  examination  of  the  seven  permitted  colors,  1907 179 

Need  of  chemical  control 179 

First  met  hods  of  analysis  used 181 

Moid  ure 182 

Chlorin  aschlorids L82 

Sulphated  ash 182 

Total  sulphur 183 

Gut /.cit  lest 183 

Heavy  metals 183 

Total  insolubles 184 

lit  Imt  extractive 184 

Results  of  chemical  examination,  1907 184 

Detailed  chemical  data  on  each  permitted  color 184 

Recalculation  of  analytical  data  on  basis  of  coloring  matter  pres- 
ent    187 

Market  quality  of  the  seven  permitted  colors 190 


CONTENTS.  7 

Page. 

XV.  Guides  in  determining  degree  of  purity  and  cleanliness 192 

XVI.  Analyses  of  certified  lots  of  permitted  colors,  1Q09-10 198 

Tabulation  of  results 198 

Comparison  of  analyses  made  in  1907 201 

Conformity  of  analytical  data  with  theoretical  composition 202 

Arsenic  determinations  on  86  batches 204 

Suggested  requirements  for  certified  colors 205 

XVTI.  Methods  of  analysis  used  in  testing  colors  for  certification 210 

Introduction 210 

Xaphthol  Yellow  8 211 

Ponceau  3R 215 

Orange  I 217 

Amaranth 220 

Light  Green  S  F  Yellowish 221 

Erythrosin 222 

Indigo  disulphoacid 

XVm.  Addenda 

Additional  examination  of  coal-tar  dyes 

Supplementary  list  of  trade  names  of  coal-tar  colors 

XIX.  Index  of  authorities  quoted 227 


ILLUSTRATION 


Page. 
Fig.  1.  Apparatus  used  in  the  determination  of  arsenic 213 


Digitized  by  the  Internet  Archive 
in  2013 


http://archive.org/details/tarfosuseOOhess 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


INTRODUCTION. 
PURPOSE  OF  THE  INVESTIGATION. 

For  the  purposes  of  the  investigation  reported  in  the  following  pages, 
the  legitimacy  of  the  coloring  of  food  and  food  products  under  certain 
conditions  is  regarded  as  established;  the  ethical  and  dietetic  aspects 
of  the  question  of  food  coloring  are  not  here  considered. 

The  means  at  hand  for  coloring  food  products  may  be  conveniently 
classified  as  vegetable,  animal,  mineral  or  inorganic,  and  synthetic 
or  so-called  coal-tar  colors  or  dyes.  Representatives  of  each  of  these 
have  at  one  time  or  another  all  been  used  in  the  coloring  of  food,  and 
the  laws  of  various  European  and  American  States  have,  from  time 
to  time  prohibited  the  use  of  certain  specified  members  or  all  of  each 
or  some  of  the  foregoing  classes.  It  is  therefore  obvious  that  even 
for  the  legitimate  purposes  for  which  food  can  be  colored,  improper 
means  are  at  command,  and  some  of  these,  if  not  all,  have  been 
prohibited  by  law  at  some  time  or  another. 

It  is  the  function  of  the  present  work  to  determine  what  members 
of  the  synthetic  or  coal-car  colors  should  be  considered  legitimate 
for  coloring  fond-.  It  is  confidently  believed  that  the  material 
collected  in  the  following  pages  point-  clearly  and  solely  to  the 
following  conclusions: 

1.  Coal-tar  dyes  should  not  be  used  indiscriminately  in  foods. 

2.  Onrj  specified  coal-tar  dyes  should  be  used  in  foods. 

3.  Only  tested  and  certified  dyes  should  he  used  in  food-. 

The  work  here  reported  has  Furnished  the  basis  for  Food  [nspection 
Decisions  Nbs.  76,  77,  and  106,  issued  duly  13,  L907,  September  -J."). 
i(.i<>7.  and  March  25,  L909,  respectively,  and  the  investigation  it-elf 

was   practically   terminated  January    1.    1910. 

The  effect  of  these  decisions  ha-  been  to  restrict  the  coal-tar  colors 
permitted  for  use  in  food-  to  seven  specified  and  enumerated  colors, 
until  Buch  time  as  it  -hall  he  -how n  with  reasonable  conclusiveness 

that  other  Colors  Bhould  be  added  to  BUch  li-t  :  and  further,  all  coal-tar 

colors  permitted  for  use  in  food  are  to  be  of  a  degree  of  purity  and 

cleanliness  acceptable  to  the   Department   of  Agriculture,  and  are  to 

be  -o  certified. 

o 


10  COAL-TAR  COLORS  USED  IX   FOOD  PRODUCTS. 

In  order  to  avoid  any  uncertainty  as  to  the  chemical  composition 
of  the  enumerated  colors,  direct  reference  is  made  in  Food  Inspection 
Decision  No.  7G  to  a  standard  work  in  which  such  chemical  composi- 
tion is  clearly  and  unequivocally  set  forth.  The  relevant  parts  of 
Food  Inspection  Decision  Xo.  76  are  as  follows: 

The  use  of  any  dye,  harmless  or  otherwise,  to  color  or  stain  a  food  in  a  manner  whereby 
damage  or  inferiority  is  concealed  is  specifically  prohibited  by  law.  The  use  in  food 
for  any  purpose  of  any  mineral  dye  or  any  coal-tar  dye,  except  those  coal-tar  dyes 
hereinafter  listed,  will  be  grounds  for  prosecution.  Pending  further  investigations 
now  under  way  and  the  announcement  thereof,  the  coal-tar  dyes  hereinafter  named, 
made  specifically  for  use  in  foods,  and  which  bear  a  guaranty  from  the  manufacturer 
that  they  are  free  from  subsidiary  products  and  represent  the  actual  substance  the 
name  of  which  they  bear,  may  be  used  in  foods.  In  every  case  a  certificate  that  the 
dye  in  question  has  been  tested  by  competent  experts  and  found  to  be  free  from 
harmful  constituents  must  be  filed  with  the  Secretary  of  Agriculture  and  approved 
by  him. 

The  following  coal-tar  dyes  which  may  be  used  in  this  manner  are  given  numbers, 
the  numbers  preceding  the  names  referring  to  the  number  of  the  dye  in  question  as 
listed  in  A.  G.  Green's  edition  of  the  Schultz-Julius  Systematic  Survey  of  the  Or- 
ganic Coloring  Matters,  published  in  1904. 

The  list  is  as  follows: 

Red  shades:  107.  Amaranth.     56.  Ponceau  3  R.     517.  Erythrosin. 

Orange  shade:  85.  Orange  I. 

Yellow  shade:  4.  Naphthol  Yellow  S. 

Green  shade:  435.  Light  Green  S  F  Yellowish. 

Blue  shade:  692.  Indigo  disulfoacid. 

Each  of  these  colors  shall  be  free  from  any  coloring  matter  other  than  the  one 
specified  and  shall  not  contain  any  contamination  due  to  imperfect  or  incomplete 
manufacture. 

The  reasons,  broadly  considered,  which  led  up  to  these  food  inspec- 
tion decisions  are  given  in  concise  fashion  in  this  introduction. 

Looking  over  the  restrictions  placed  upon  coal-tar  colors  by  the 
lawmakers  of  the  various  countries  it  will  be  found  that  certain 
colors  are  in  some  instances  specifically  prohibited  and  in  other 
instances  that  certain  specific  colors,  or  classes  of  colors,  and  only 
such,  are  permitted  for  the  legitimate  purposes  of  food  coloring. 

Private  organizations,  such  as  the  Swiss  Society  of  Analytical 
Chemists  and  the  National  Confectioners'  Association  in  the  United 
States,  have  also  made  recommendations  permitting  specific  colors 
only,  and  in  addition  specifically  prohibiting  others.  Individual 
authors  have  likewise  made  similar  recommendations.  The  control 
of  the  quality  of  llio  food  colors  practiced  on  the  part  of  those  Gov- 
ernments which  restrict  the  use  of  coal-tar  colors  to  certain  individ- 
uals, so  far  as  any  publications  show,  has  not  been  very  extensive. 

The  action  taken  against  the  use  of  coal-tar  colors  for  food-coloring 

purposes  has  ranged  all  the  way  from  absolute  prohibition  of  their 

Use  for  any   purpose  whatsoever  to  the  practically  unlimited   use  in 

Legitimate  food  coloring  operations  of  all  but  two  of  such  colors. 


INTRODUCTION.  11 

Intermediate  between  these  two  extremes  we  find  the  prohibition  of 
a  greater  number  than  two,  or  of  all  the  members  of  this  class  except 
certain  specified  colors,  and  even  here  with  the  restriction  that  they 
shall  be  used  only  for  certain  legitimate  food-coloring  purposes. 

It  would  be  desirable  to  have  a  number  of  coal-tar  colors  of  estab- 
lished harmlessness  specifically  permitted,  particularly  if  the  number 
be  sufficient  to  meet  all  the  legitimate  demands  arising  in  the  food- 
coloring  art.  To  prohibit  only  specified  coal-tar  colors  and,  by 
implication,  to  permit  all  the  rest  of  this  class,  would  allow  the 
unrestricted  use  of  newly  discovered  colors,  and  all  other  coal-tar 
colors  not  examined  as  to  their  effect  on  health.  A  limited  list  of 
permitted  coal-tar  colors  which  would  make  the  use  of  all  coal-tar 
colors  outside  of  the  permitted  list  illegal  would  properly  protect 
the  health  and  could  work  no  substantial  hardship  upon  those 
engaged  in  food  coloring.  Any  such  hardship  would  be  avoided  by 
providing  that  if  it  is  shown  that  none  of  the  colors  of  the  permitted 
list  meets  certain  legitimate  requirements  and  that  coal-tar  colors 
outside  the  permitted  list  are  capable  of  satisfying  this  need  and  are 
in  and  of  themselves  harmless  the  permitted  list  can  be  expanded  by 
the  proper  authorities  to  meet  additional  needs  or  growing  require- 
ments without  exposing  the  public  health  to  any  risk. 

NUMBER  OF  COLORS  PERMITTED. 

It  will  be  shown  in  the  following  pages  that  in  the  summer  of  1907 
there  were  on  the  market  of  the  United  State-  80  different  chemical 
individuals,  or  so-called  coal-tar  colors,  offered  for  the  coloring:  of 
food.  It  has  been  known  since  1888  that  it  is  unsafe  to  attempt 
to  predict  the  harmfulness  or  the  harmlessness  of  coal-tar  colors  by 
inference  or  analogy;  therefore  an  ideally  perfect  permitted  list  should 
contain  only  such  colors  as  have  each  been  examined  physiologically, 
separately,  and  specifically,  and  their  harmlessness  determined  by 
actual  test.  Out  of  the  80  colors  referred  to  30  had  not  been  exam- 
ined at  all,  so  far  as  the  literature  shows,  and  therefore  their  harm- 
leasnesfl  is  certainly  open  to  question;  20  had  been  examined  physi- 
ologically! and  the  published  accounts  with  respect  to  their  harm- 
lessness or  their  harmfulness  are  in  each  case  contradictory;  on  8 
none  but  adverse  reports  were  to  be  found  in  literature.  Leaving 
only  16  out  of  80  colors  on  the  market  which  had  been  established 
with  more  or  less  certainty  a-  harmless-  that  is,  the  users  of  these  s 

Colors  were  deliberat ely  taking  chance-  with  the  public  health,  since 

the  harmful  nature  of  those  8  had  for  a  long  time  past  been  known  to 
those  conversant  with  such  subjects;  the  use  of  the  26  doubtful 
colors  is  more  defensible  than  the  use  of  the  s  known  to  be  harmful. 

Out  of  the  30  of  whose  action  nothing  was  known  it  can  not  he  -aid 


12  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

how  many  are  or  are  not  harmful,  nor  can  the  risk  forced  upon  the 
public  health  be  satisfactorily  measured. 

This  brief  summary  must  suffice  for  the  present  as  a  justification 
for  the  restrictions  of  the  permitted  colors  to  7  in  number.  The  full 
reasons  for  each  and  every  step  will  appear  in  their  proper  places  in 
the  pages  following. 

QUALITY  AND  EFFICIENCY  OF  COLORS  PERMITTED. 

An  examination  of  30  specimens  representative  of  the  7  selected 
permitted  colors  on  the  United  States  market  in  the  summer  of 
1907  disclosed  such  a  condition  of  uncleanliness  of  product,  or  care- 
less or  improper  manufacture,  and  the  use  of  such  utterly  inferior 
qualities  of  products  for  food  coloring  purposes,  that  control  over 
the  quality  of  the  seven  permitted  colors  seemed  necessary.  The 
results  of  the  work  in  the  making  and  maintaining  of  standards  of 
quality  for  each  of  these  seven  colors  also  justify  this  control.  That 
there  was  in  1907,  and  for  a  year  or  more  later,  a  considerable  diver- 
gence of  opinion  among  chemists  as  to  what  should  be  the  proper 
quality  requirements  for  these  colors  is  shown  by  the  fact  that  out 
of  72  foundation  certificates  offered  in  accordance  with  Food  Inspec- 
tion Decisions  Nos.  76  and  77,  57  were  rejected  on  their  face  because 
they  did  not  comply  with  the  standards  of  quality  then  in  mind, 
or  then  shown  to  be  commercially  attainable.  Much  objection  has 
been  made  by  many  of  those  whose  certificates  were  rejected  on  the 
ground  that  the  standards  then  in  mind  were  unreasonable,  unjusti- 
fiable, and  nonattainable.  The  actual  results,  however,  are  that 
with  very  few  exceptions  the  standards  in  mind  early  in  the  work 
have  all  been  exceeded  in  practice;  the  41,000  pounds  (20.5  tons) 
of  certified  colors  now  in  existence  made  in  97  batches,  or  an  average 
of  more  than  420  pounds  per  batch,  are,  with  the  exception  of  perhaps 
one  or  two  first  batches,  far  cleaner  than  was  expected  when  the  57 
certificates  above  referred  to  were  rejected. 

There  has  been  no  complaint  against  the  permitted  colors  for  want 
of  efficiency  or  for  the  possession  of  unsuitable  attributes,  which  1ms 
been  pressed  or  sustained  with  any  such  earnestness  as  would  rea- 
sonably be  expected  if  the  defects  complained  of  were  as  great  as 
they  were  represented.  Complaints  have  been  made  against  (he 
yellow,  when  used  in  acidulated  fruit  sirups,  on  account  of  its  pos- 
sessing a  bitter  taste;  the  proof  of  this,  so  far  as  any  lias  been  offered, 
was  for  a  long  time  not  of  a  convincing  nature,  and  it  was  two  years 
after  the  first  objection  was  raised  before  any  concerted  or  positive 
action  was  taken  by  those  interested.  The  yellow  has  also  been 
criticized  because  it  is  not  sufficiently  fast  to  light ;  although  it  was 
satisfactorily  shown  that  another  yellow  was  faster  to  light  than  the 
permitted    yellow,    no   one   has   maintained    that   the  yellow   desired 


INTRODUCTION.  13 

was  actually  preferable  to  the  permitted  yellow  wholly  and  solely 
because  of  its  superior  fastness  to  light. 

The  blue  has  been  criticized  because  it  is  not  of  the  proper  shade 
to  permit  of  its  use  in  the  bluing  of  sugar,  but  the  substitute  offered 
therefor  has  not  been  supported  by  its  sponsors  in  a  way  to  indicate 
that  a  defect  of  serious  magnitude  exists.  On  the  grounds  of  suffi- 
ciency and  of  efficiency  the  fist  of  permitted  colors  selected  appears 
to  have  been  justified  by  the  absence  of  any  real  or  substantial  com- 
plaint against  them,  on  either  or  both  of  these  grounds,  during  a 
period  of  more  than  three  years. 

None  of  the  seven  permitted  colors  is  patented;  their  manufacture 
and  their  purification  are  open  to  all,  and  none  of  the  80  colors  on 
the  market  in  the  summer  of  1907,  with  perhaps  one  exception,  had 
been  discovered  since  1891;  in  other  words,  the  advances  in  the  coal- 
tar  industry  from  1891  to  1907  had  added  nothing  to  the  colors 
serviceable  to  the  art  of  food  coloring. 

The  list  of  colors  permitted  in  Food  Inspection  Decision  Xo.  76 
embraces,  therefore,  a  sufficient  number  of  colors  for  all  legitimate 
food-coloring  purposes,  the  coloring  of  fats,  oils,  butter,  etc.,  excepted, 
for  which  no  suitable  color  had  been  examined  and  reported  in  the 
literature  as  being  harmless  and  fit  for  use  in  foods;  they  can  be  made 
by  any  one;  no  one  can  have  a  monopoly  in  any  one  of  them  by 
virtue  of  patents;  any  competent  maker  can  make  all  or  any  of 
them  and  purify  them  to  the  required  degree  of  cleanliness.  The 
standards  growing  out  of  the  control  exercised  by  the  Department  of 
Agriculture  are  such  as  to  insure  that  the  colors  used  for  food-coloring 
purposes  possess  a  proper  degree  of  cleanliness  and  such  a  degree  of 
cleanliness  is  commercially  feasible  and  is  a  commercial  reality. 

The  policy  adopted  in  this  respect  is  therefore  justified  not  only 
from  the  viewpoint  of  the  history  of  the  attempts  on  the  part  of 
various  governments  to  control  the  quality  of  food  colors,  hut  also 
by  the  results  actually  obtained  by  its  adoption.  This  policy  of 
restricting  food  colors  to  certain  chemical  individuals  and  demand- 
ing that  those  possess  certain  qualities  is  in  complete  harmony  with 
the  following  suggestion  made  to  the  commission  on  rules  and  regu- 
lations under  the  food  and  drugs  act,  at  its  hearing  in  New  York, 
in  September,  1906. 

Any  kind  of  a  harmless  color  should  !><•  permitted,  provided  ii  is  not  a  color  generally 
known  n>  he  poisonous,  ox  generally  found  t"  be  poisonous,  or  one  that  may  be  almost 
impossible  to  !„■  produced  without  continuing  son  a-  poison  within  itself  when  finished 

and  ready  for  use.  Coal-tar  colors,  as  a  class,  should  not  be  prohibited,  but  all  those 
coal-tar  colors  generally  found  to  1m-  p.  [sonoUS,  I  r  which  are  hard  to  produce  without 

containing  some  poisonous  propertief  when  ready  for  use,  should  be  forbidden  the 
i)ri\  [lege  of  being  used,  or  offered  for  sale  for  use  in  food. 

Under  the  provisions  of  section  2,  we  have  this  to  recommend  to  the  commi 
that  every  person  sailing  or  using  a  coal-tar  color  in  food  or  drink,  should  be  required 


14  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

to  secure,  either  on  his  own  account,  or  from  the  person  from  whom  he  buys  such  color, 
a  certificate  to  the  effect  that  the  identical  color  used  has  been  tested  for  poisonous 
ingredients,  and  is,  to  the  knowledge  of  the  chemist  making  the  test,  absolutely  harm- 
less. The  chemist  should  be  required  to  be  a  competent  physiological  chemist,  and 
must  certify  as  above  under  oath.  This  would  mean  not  that  each  package  of  color 
would  have  to  be  tested,  but  that  every  batch  would  have  to  be  tested,  and  the 
certificate  would  then  be  held  to  relate  to  every  batch.  Such  tests  should  be  made 
in  the  United  States  and  the  chemist  certifying  should  reside  in  and  be  a  citizen  of 
the  United  States. 

It  should  not  be  deemed  sufficient  to  have  any  particular  brand  of  coal-tar  color 
tested  once,  and  a  blanket  certificate  given,  covering  the  whole  brand  as  long  as  it  may 
be  sold,  but  every  ounce  of  coal-tar  color  put  out  by  a  color  manufacturer  should  be 
shown  by  actual  test  to  be  harmless. 

While  the  exact  mode  of  reaching  the  end  in  view  is  somewhat  dif- 
ferent from  the  one  suggested  above,  yet  the  fundamental  object,  that 
each  batch  of  color  used  in  foods  shall  be  specifically  tested,  and  that 
such  colors  shall  be  harmless,  is  attained  with  reasonable  certainty; 
and  although  there  are  colors  other  than  these  seven  which  are 
undoubtedly  equally  as  little  objectionable,  and  while  it  is  true  that 
the  present  policy  contemplates  the  permitted  use  of  but  seven 
specific  colors,  yet  that  policy,  as  before  outlined,  is  sufficiently  broad 
and  elastic  to  enable  the  addition  of  a  color  to  the  permitted  list, 
when  it  is  shown  that  such  color  really  fills  a  need,  not  properly  satis- 
fied by  one  of  the  colors  already  permitted  or  some  combination  of 
these,  and  is  in  and  of  itself  harmless.  There  can  be  no  objection  to 
the  expansion  of  the  list  to  such  an  extent  as  to  include  every  harmless 
coal-tar  color  in  existence;  but  the  burden  of  proving  such  real  need 
and  harmlessness  is  very  properly  placed  upon  those  who  are  seek- 
ing such  expansion. 

As  far  back  as  1892  the  following  statement  was  made  on  page  IV 
of  the  Leffmann  translation  of  Weyl's  book  on  coal-tar  colors,  in  con- 
nect ion  with  the  various  European  legislative  enactments:  "It  is 
certain  that  none  of  these  plans  is  even  approximately  satisfactory 
and  the  problem  will  be  even  more  difficult  of  solution  in  the  United 
States;  indeed,  it  seems  to  me  to  be  unsolvable."  In  view  of  this 
opinion  the  results  of  the  food  inspection  decisions  as  herein  shown 
may  properly  be  regarded  as,  at  least,  a  step  in  the  right  direction 
tow  ard  I  lie  solution  of  this  problem. 

This  opinion  Is  further  supported  by  C.  A.  Neufeld  who,  in  review- 
ing Food  [nspection  Derision  No.  76,  says:  "The  idea  of  permitting 
only  specific  selected  coloring  matters  for  use  in  the  production  of 
articles  of  \'<>o(\,  and  of  excluding  all  other  colors  from  such  uses,  must, 

in  the  interest  of  control  of  articles  of  food,  be  regarded  ai  an  extra- 
ordinarily happy  one;  a  similar  regulation  is  to  be  urgently  recom- 
mended lor  our  own  country."  (Zts.  Nalir.  Oenussm.,  1908,  v.  15, 
p.  W.) 


IDENTITY   OF   COAL-TAR   COLORS,   1907.  15 

IDENTITY  OF  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS  IN 
THE  UNITED  STATES  IN  1907. 

COLLECTION  OF  SAMPLES. 

The  question  "  Which  coal-tar  colors  shall  be  permitted  for  use  in 
coloring  such  food  products  as  are  to  be  consumed  within  the  United 
States?"  can  be  answered,  "All  colors  now  in  use,  or  to  be  used  for 
that  purpose,  provided  they  are  harmless  and  necessary  as  defined  on 
page  14." 

This  involves  the  further  questions : 

1.  Which  coal-tar  colors  of  the  695  different  chemical  individuals 
now  on  the  world's  markets  are  actually  used  in  the  United  States  for 
that  purpose  ? 

2.  If  restricted  to  such  coal-tar  colors  as  are  now  in  use  in  the 
United  States  for  this  purpose,  would  this  be  likely  to  hamper  or  inter- 
fere with  the  invention  of  other  coal-tar  colors  suitable  for  the 
coloring  of  food  ? 

It  would  be  physically  impossible  to  go  to  every  user  of  coal-tar 
colors  in  food  products  in  the  United  States  and  obtain  specimens  of 
the  coal-tar  colors  so  employed;  this  would  be  impracticable  not  only 
because  of  the  large  number  of  such  users,  and  their  wide  geographical 
distribution,  but  also  because  they  often  do  not  know  what  they  arc 
using,  and  further  because  of  a  reluctance,  undoubtedly  to  be  encoun- 
tered among  many,  to  disclose  the  nature  of  the  products  employed. 
This  is  rendered  more  than  likely  by  the  attitude  of  some  of  the 
makers  of  coal-tar  colors,  or  their  accredited  agents,  as  will  be  shown 
Later. 

However,  the  sources  of  coal-tar  colors  are  limited  in  number.  By 
reference  to  panes  IX  and  X  of  "A  systematic  survey  of  the  organic 
coloring  matters/'  by  Arthur  G.  Green,  published  in  London  and  New 
York  by  Macmillan  &  Co.  (Ltd.),  in  1904  (hereinafter  referred  to  as 
"Green  Tables"),  it  will  be  seen  that  there  are  approximately  37 
different  concerns  t  be  world  over  engaged  in  the  manufacture  of  coal- 
tar  colors.  Therefore  a  canvass  of  these  sources  for  such  coal-tar 
colors  as  in  their  judgment,  or  in  their  business  practice,  they  regard 

as  proper  for  USC  in  I"<mm|  product >,  is  the  best  way  of  arriving  at  a  fair 

demarcation  of  the  held  of  coal-tar  colors  bere  in  question. 
Communication  was  therefore  had  with  13  actual  manufacturers  of 

coal-tar  colors,    in   an   endeavor   to   obtain    from   them   BUch   coal-tar 

colors  as  in  their  judgment  or  business  practice  are  suitable  loin 
are  used  in  food  products. 

A  request  was  also  made  for  information  as  to  the  chemical  com- 
position of  t he  coal-tar  col<>r  specimens  submitted j  in  order  to  avoid 
confusion,  it  was  further  asked  that  reference  be  made  to  the  Green 

Tables,   in   which  each  chemical   individual  or  coal-tar  color  ha-  its 


16 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 


own  number,  and  if  any  of  the  contributed  specimens  was  not  so  listed 
that  the  chemical  composition  be  stated  in  a  manner  analogous  to 
that  used  in  the  Green  Tables.  This  procedure  was  necessary  in 
order  to  reduce  the  terminology  to  a  common  and  nonequivocal  basis. 
Out  of  the  13  makers,  or  their  accredited  sole  importers  or  selling 
agents  in  the  United  States,  who  were  consulted,  9  have  supplied  the 
specimens  requested;  the  remaining  4  promised  to  contribute,  but 
have  not  done  so.  In  the  following  table  is  shown  the  amount  and 
character  of  the  information  obtained: 

Tabulation  of  distribution  of  replies  and  character  of  information  received. 


Geographical  distribution. 

Number 
of 

samples 
contri- 
buted. 

Number 

of 
samples 
referred 

to 
Green 
Tables. 

Number 

of 
samples 

not 
referred 

to 
Green 
Tables. 

No 

Country. 

Coal-tar 
color 

makers. 

Makers- 
asked 
to  send 
samples. 

Makers 

not 
sending 
samples. 

Makers 
sending 
samples. 

composi- 
tion or 
ambigu- 
ous ter- 
minology. 

Germany 16 

6 
1 
1 
3 
2 

6 

1 

181 
12 

106 
12 

1 

74 

England 8 

France 5 

1 
3 

Switzerland... 

5 
1 

2 

51 

35 

5 

21 

Holland 1 

Belgium 

Total 

37 

13 

4 

9 

254 

153 

6 

95 

In  order  to  make  provision  for  the  24  makers  listed  in  the  Green 
Tables  and  not  included  in  the  13  makers  addressed  requests  for 
samples  were  sent  to  two  domestic  houses  which  import  coal-tar  colors 
from  scources  other  than  the  above,  for  use  in  food  products;  their 
products  must  fairly  represent  any  of  the  colors  not  covered  by  the 
13  makers  addressed.  Of  these  two  importers,  one  responded  with 
13  samples,  and  of  each  he  gave  the  number  in  the  Green  Tables 
corresponding  to  each  specimen;  the  other  importer  has  not  redeemed 
his  promise  to  contribute  specimens. 

A  third  importer  volunteered  the  Green  Table  numbers  of  hair  out 
of  five  coal-tar  colors  used  in  his  business,  but  could  not  even  approx- 
imately say  what    the  remaining  color  was  chemically.      He  did  Q01 

contribute  any  specimens,  nor  was  that  necessary  ;it  the  time  this 
informatioD  was  volunteered. 

A  fourth  importer  contributed  specimens  of  five  coal-tar  colors 
needed  in  his  business,  but  was  able  to  give  Green  Table  numbers  for 
only  three  of  them:  he  could  not  give  eves  approximately  the  chem- 
ical composition  of  the  remaining  two. 

Out  of  the  17  responsible  concerns  consulted  5,  or  29  percent,  have  not 
found  it  to  their  interest  to  contribute  either  specimens  or  information. 


IDENTITY   OF    COAL-TAR    COLORS,    1907. 


17 


CLASSIFICATION  OF  SAMPLES  SUBMITTED. 
GREEN    TABLE    NUMBERS. 

Out  of  the  284  specimens  contributed,  or  reported  on,  172  (60.6 
per  cent)  were  identified  as  to  their  chemical  composition,  by  refer- 
ence to  the  Green  Tables;  6  (2.1  per  cent)  were  otherwise  unequivo- 
cally identified  chemically,  and  for  106  (37.3  per  cent)  the  makers, 
or  their  responsible  agents,  declined  to  state  the  chemical  composi- 
tion, i.  e.,  62.8  percent  were  unequivocally  identified,  and  the  remain- 
ing 37.3  per  cent  were  not  so  identified. 

The  specimens  submitted  are  therefore  divisible  into  the  following 
three  classes: 

Class  I.  Those  for  which  numbers  were  given  in  the  Green  Tables, 
numbering  172. 

Class  II.  Those  whose  composition  was  given  in  chemical  language, 
numbering  6. 

Class  III.  Those  whose  composition  was  not  given  in  any  lan- 
guage capable  of  correct  and  certain  translation  into  chemical  terms, 
numbering  106. 

Consider  Class  I.  The  Green  Tables,  page  VI,  divide  the  coal-tar 
colors  into  21  groups,  comprising  695  different  chemical  individual 
coal-tar  colors.  The  172  members  of  Class  I  number  in  all  74  indi- 
viduals, or  10.6  per  cent  of  the  Green  Tables,  and  fall  into  11  of  the 
21  groups  of  those  Tables. 

The  following  table  classifies  the  samples  according  to  the  Green 
Table  groups: 

Green  Table  groups  and  number  of  collected  samples  falling  within  (hen}. 


Color  groups  of  the 
Green  Tables. 

Number 
of  mem- 
bers   in 
group. 

Collected    samples 
falling    into    the 
several  groups. 

Color  groups  of  the 
Ben  Tables. 

Number 
of  mem- 
bers in 
group. 

Collected     samples 
falling    into    the 
several  groups. 

Number. 

Percent. 

Number. 

Percent 

Nitro 

204 

11 
5 

1- 

-' 

U 

l 

30 
11 

l»i 

24 
5 

Anthracene 

Indopbeool 

37 

38 

32 

9 

) 
21 

7 

2 

5 

■ 

Tctruk  i-.:/.o 



2 

1 

20 



Btllbene 

1 

tone 

Sulphld.. 

Diphenj  Imethane.. 
Triphciix  Imethane. 
Xanthene 

1 

i:> 
9 

H 

Iildi^u 

1 

i:. 

74 

Acri.lm.... 

97291c      r.ull.  147—12- 


18 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 


SOURCE. 

The  distribution  of  the  74  different  chemical  individuals  of  Class  I 
among  the  12  different  sources  from  which  they  were  obtained  is  as 
follows : 

Distribution  of  the  74  different  samples  of  Class  I  among  the  12  sources  supplying  same. 


Number. 

Percent. 

Number 
of  sources 
from 
which 
each 
came. 

Number. 

Per  cent. 

Number 
of  sources 
from 
which 
each 
came. 

35 

20 

i 

4 
5 
3 

47.3 

27 
5.4 
5.4 
8.1 
2.7 

1 
2 
3 
4 
5 
6 

1 

1 

0 
1 

0 
0 

1.35 
1.35 

7 
8 
9 
10 
11 
12 

1.35 

It  follows  from  this  table  that  there  is  very  little  unanimity  among 
the  different  concerns  furnisliing  coal-tar  colors  for  use  in  food  prod- 
ucts as  to  which  of  their  products  are  desirable,  necessary,  or  suitable 
for  such  use. 

Inspection  of  this  table  shows  that  only  three  colors  out  of  74, 
or  4  per  cent,  were  wanted  by  more  than  half  of  all  the  sources;  that 
only  6,  or  8.1  per  cent,  were  wanted  by  half  of  the  sources;  and  that 
not  one  of  the  colors  was  wanted  by  all  the  sources.  This  last  state- 
ment is  true  of  manufacturers  as  well  as  importers,  each  group  taken 
by  itself. 

PATENTS. 

This  lack  of  unanimity  is  not  due  to  the  patent  situation,  because 
not  more  than  one  of  these  74  products  is  patented,  and  it  is  more 
than  likely  that  the  United  States  patent  on  this  product  has  long 
since  expired. 

Moreover,  only  6  of  the  12  sources  offered  colors  at  one  time 
patented  by  themselves  or  others.  The  total  number  of  such  ex- 
patented  products  is  45,  and  of  these  only  22  were  offered  by  those 
who  had  patented  them;  the  remaining  23  were  offered  by  sources 
other  than  the  ex-pat  cut  ees,  and  were  not  offered  by  such 
ex-patentees. 

Patented  colors. 


IDENTITY   OF    COAL-TAR    COLORS,    1907. 


19 


It  would,  therefore,  seem  to  be  rather  clear  that  others  think  more 
favorably  of  such  ex-patented  products  as  food  colors  than  do  the 
original  patentees.  In  view  of  the  fact  that  the  latter  would  generally 
be  in  a  better  position,  and  would  have  greater  opportunity  than  any 
one  else  to  judge  of  the  suitability  of  the  patented  products  for  use 
in  food  products,  it  may  well  be  inferred  that  such  products  are  not 
altogether  free  from  disadvantages  as  food  colors. 

The  second  of  the  two  questions  propounded,  namely,  If  restricted 
to  such  coal-tar  colors  as  are  now  in  use  in  the  United  States  for  tins 
purpose,  would  this  be  likely  to  hamper  or  interfere  with  the  invention 
of  further  coal-tar  colors  suitable  for  the  coloring  of  food  products? 
can  be  answered  "No"  because  none  of  the  colors  submitted  was 
discovered  later  than  1891;  out  of  the  214  coal-tar  colors  since  then 
discovered  not  one  was  among  those  submitted  for  use  in  foods,  and 
out  of  the  481  discovered  in  1891  and  prior  thereto,  only  74  were  so 
submitted,  or  2  out  of  every  13  of  such  colors.  In  the  following 
table  these  data  are  given  year  by  year: 

Coal-tar  colors  discovered  from  1740  to  1891. 


Year 
of  dis- 
covery. 

Num- 
ber of 
sub- 
mitted 

colors 
discov- 
ered. 

Total 
num- 
ber of 
coal- 
tar 
colors 
discov- 
ered. 

Year 
of  dis- 
covery. 

Num- 
ber of 
sub- 
mitted 
colors 
discov- 
ered. 

Total 
num- 
ber of 
coal- 
tar 
colors 
discov- 
ered. 

Year 
of  dis- 
covery. 

Num- 
ber of 
sub- 
mitted 
colors 
discov- 
ered. 

Total 
num- 
ber of 
coal- 
tar 
colors 
discov- 
ered. 

Year 
of  dis- 
covery. 

Num- 
ber of 
sub- 
mitted 
colors 
discov- 
ered. 

Total 
num- 
ber of 
coal- 
tar 
colors 
discov- 
ered. 

1740 
1856 
1859 
1861 
1862 
1863 
1867 

1 

1 
1 
•-' 
1 
1 
1 

1 

a 

i 

3 
5 
3 
3 

Is71 
\s~\ 
1^7.5 

is:»; 
1877 

1878 
1879 

1 
6 
5 

■J 
12 

7 

r> 
4 
12 
9 
10 
26 
23 

1881 
1882 
1883 
1884 

1885 
1886 

4 
5 
9 
3 
2 
3 

11 
20 
25 
16 
21 
32 

1887 

1888 
L89Q 
1891 

Total. 

3 

29 
36 
46 
33 

74 

378 

SHADES    OF    COLOR. 


The  sufficiency  of  the  7  1  colors  u>o<l  for  food-coloring  purposes  in 
the  United  States,  for  any  and  nil  tinctorial  ranges,  no  matter  how 
refined,  appears  from  the  following  table: 

tubmitUd  colors  thawing  thadu  end  number  of  sources 
tupp&ying  each. 


I'iea. 

Number  of  sources  out  of  a  possible  12  Offering  MOfi  color. 

Total 

number 

1 

•_> 

3 

1 

5 

7 

Q 

ID 

of  ilycs 

offered 

fur  cub 

■had*. 

UN 
106 

1.^ 

11', 

lOfl 

UN 

1H7 

u 

20  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

Green   Table  numbers  of  the  74  submitted  colors  showing  shades  and  number  of  sources 

supplying  each — Continued. 


Number  of  sources  out  of  a  possible  12  offering  each  color. 

Total 
number 

Shades. 

1 

2 

3 

4 

5 

6 

7 

8 

9 

10 

of  dyes 
offered 
for  each 
shade. 

502 
518 
520 
523 

512 

448 

504 
517 

7 

54 

516 

53 

64 

56 

89 
269 
329 

9 

Yellowish  red 

3 

Scarlet 

55 

3 

1 

Yellow 

510 

8 

94 

4 

7 

Reddish  yellow 

84 
14 

17 
85 
95 

650 

2 

13 

2 

667 

18 
97 

439 
476 
480 
655 

440 

468 

464 

287 

433 
434 

425 

2 

Orange 

86 

6 

Blue 

692 

6 

Green  blue 

, 

Violet 

452 

451 

3 

, 

Green 

398 

435 

4 

427 

x 

428 

1 

101 
137 
139 

8 

201 

197 

188 
601 

, 

BltW  to  bluish  r«'<l   to   violet. 



10 

49 

11 

4 

Total 

35 

20 

4 

1 

5 

3 

1 

1 

1 

74 

The  six  colors  comprising  Class  II  (those  not  listed  in  fche  Green 

Tables   but   whoso   composition  was   avowed    OT   disclosed)    are   one 

black,  one  yellow,  and  one  orange  among  tin4  water-soluble  colors, 
and  three  yellows  among  the  water-insoluble  colors.  Therefore  two- 
thirds  of  fche  United  States  market  as  thus  disclosed  calls  for  a  total 


IDENTITY   OF   COAL-TAR   COLORS,   1907. 


21 


of  80  different  chemical  individuals,  of  which  73  are  water-soluble  and 
7  are  water-insoluble  and  are  used  as  oil  or  fat  colors.  The  remain- 
ing third  of  the  makers  or  dealers  either  do  not  possess  the  information 
or  are  unwilling  to  give  it.  Xo  attempt  has  yet  been  made  to  enter 
systematically  into  this  unknown  region,  but  careful  examination 
warrants  the  belief  that  it  can  add  nothing  of  material  value  to 
the  data  already  obtained  which  show  a  total  of  23  shades  for  the 
73  water-soluble  coal-tar  colors,  summarized  as  follows: 


X  umber  of  coal-tar  colors. 


5  red  shades 26 

4  yellow  shades 14 

1  orange  shade 7 

2  blue  shades 7 

3  violet  shades 5 


3  green  shades 

2  brown  shades 

1  blue-black  shade. . . 

1  black  shade 

1  blue  to  violet  shade. 


The  water-insoluble  colors  numbering  7  are  not  included,  but  will 
be  treated  separately  (p.  159). 

This  view  of  the  state  of  the  United  States  market  at  or  about  the 
middle  of  the  year  1907  is  without  question  a  true  reflection  of  that 
market  as  far  as  it  goes  and  the  actual  extent  of  the  coal-tar  color 
market  beyond  those  covered  by  this  canvass  of  it  is  not  likely  to  be 
very  great.  In  support  of  this  view  is  the  interchangeable  treatment 
of  formerly  patented  products,  the  great  lapse  of  time  since  a  new  food 
color  was  discovered,  and  the  fact  that  out  of  the  74  colors  submitted 
and  contained  in  the  Green  Tables  only  23  are  now  less  than  25  years 
old,  and  none  is  less  than  16  years  old. 

All  the  Green  Table  numbers  and  the  aumber  of  sources  out  of  a 
possible  12  offering  them  are  given  in  the  following  table: 

Number  ofiourcet,  out  of  a  potriblt  ttt  offering  colors  detignated  in  IS 


Qroeo 

Oreeo 

Or»  a 

Table 

Sources. 

Table 

Sources.       Table 

Booms, 

Sources. 

10 

- 

240 

1 

1 

1 

l 

480 

1 

0 

i 

M 

1 

l 

2 

10 

l 

a 

i 

;» 

11 

a 

B10 

4 

101 

;i 

11 

3 

103 

a 

1 

17 

mi 

i 

5 

ia 

l 

108 

i 

2 

l 

i 

-' 

l 

101 

» 

2 

M 

1 

ins 

i 

1 

■_• 

i 

601 

l 

ff 

1 

Its 

4 

2 

1 

1 

1 

1 

Ins 

a 

:i 

M 

•> 

i 

■_* 

1 

iLiiki/.e.l  Bfurei  in  ;  psnnlttsd  bj  P.I.  D.  ■• 


22 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Xine  manufacturers  sent  261  specimens,  an  average  of  29  each, 
distributed  as  follows:  70;  38;  20;  20;  15;  43;  25;  18,  and  12.  Two 
importers  sent  5  specimens  each,  and  one  13,  a  total  of  23  specimens, 
and  an  average  of  8.  These  figures  reflect  a  diversity  of  opinion  as 
to  what  is  needful  for  food  coloring,  since  each  one  of  these  12  makers 
or  importers  believed  that  for  all  practical  food-coloring  purposes 
his  selection  was  complete  and  sufficient. 

Classifying  the  284  specimens  as  red,  yellow,  brown,  orange,  blue, 
green,  violet,  and  black,  the  following  table  is  obtained  showing  the 
different  requirements  of  each  of  the  12  makers  or  importers  to 
produce  the  necessary  shades  of  the  eight  colors  mentioned: 

Total  specimens  submitted,  grouped  by  makers  and  colors,  showing  number  of  shades 

required  by  each. 


Maker's 
number. 

Red. 

Yel- 
low. 

Brown. 

Orange. 

Blue. 

Green. 

Vio- 
let. 

Black. 

Number 

of 
shades 
wanted 
by  each. 

Tot^.l 
speci- 
mens. 

1 

25 

10 
7 

11 
6 
4 
6 
5 
6 

13 
3 
3 

18 
6 
5 

10 
2 
3 
2 
4 
4 

10 
1 
1 

14 
2 

'"'io" 

2 

1 
..... 

2 

4 
1 
2 
5 
3 
1 
2 
1 
3 
3 
1 

2 
3 
1 

2 
4 
3 

1 
1 

5' 

5 

1 
1 

2 
2 

1 

2 
2 

1 
3 
2 

1 

i' 

..... 

7 
7 
7 
7 
7 
7 
5 
6 
6 
7 
3 
3 

70 
25 
18 
43 
20 
15 
12 
13 
20 
38 
5 
5 

2 

3... 

4 

5 

6 

7 

8... 

1 
4 
4 

1 
2 
1 



9 

10 

11 

12 

1 

Total.... 

Percent 

Maximum 

Minimum 

Average 

Permitted 

99 
34.86 
25 
3 
8.25 
3 

66 

23.  24 

18 

1 

5.50 

1 

32 

11.27 

14 

26 

9.15 

5 

22 

7.75 

5 

22 

7.75 

5 

15 

5.28 
3 

2 

0.70 

1 

2S4 
100 

2.75 

2.17 

1 

1.83 

1.83 

1 

1.25 

0.17 

From  this  table  it  appears  that  not  one  of  the  12  sources  desired  all 
of  the  8  shades  into  which  the  284  specimens  are  classifiable  to  make 
up  a  complete  set  of  food  colors;  7  out  of  the  12  sources  wanted  7  of 
the  8  shades;  2  sources  wanted  6  out  of  the  8  shades;  1  source  wanted 
5  of  the  8  shades,  and  2  sources  were  content  with  3  out  of  the  8 
shades. 

It  will  be  noticed  that  the  permitted  list  given  in   Food   Inspection 

Decision  No.  7(>  provides  for  7  dyes  covering  5  out  of  the  S  shades  of 
the  above  classification.  The  .*5  missing  shades  are  brown,  violet, 
and  black;  the  shades  provided  are  red,  yellow,  orange,  and  blue. 

It  will  also  be  noticed  thai  <>n  1  lie  whole  6  ou1  of  the  8  shades  were 
not  wanted  by  one  <>r  more  of  the  L2  sources.  The  italicized  shades 
are  the  ones  nol  provided  for  by  the  permitted  lisl  of  Food  Inspection 
Decision  No.  76. 

Brown  was  not  wanted  by  5,  nor  orange  by  1.  blue  by  3, green  by  2, 
violet  by  .*).  nor  black  by  10. 


PURPOSES   OF   POOD   COLORING.  23 

The  combinations  not  wanted  were  as  follows :  Five  sources  omitted 
black  only;  2,  brown  only;  1  blue  and  black;  1  brown  and  black;  1 
green,  violet,  and  black;  and  1  brown,  blue,  green,  violet,  and  black. 

Xot  one  of  these  12  sources  wanted  only  the  three  colors  not  found 
on  the  permitted  list,  and  2  sources  did  not  want  any  of  the  three 
missing  shades  nor  two  of  the  permitted  colors. 

In  view  of  this  large  difference  of  opinion  among  the  12  sources  as 
to  the  shades  needed  to  make  a  complete  set  of  food  colors,  the  5 
shades  selected  for  the  permitted  list  of  Food  Inspection  Decision 
No.  76  seem  reasonably  close  to  any  consensus  of  opinion  derivable 
from  the  tabulation  of  the  collected  facts. 

II.  PURPOSES  OF  FOOD  COLORING. 

The  use  of  any  color  which  conceals  inferiority,  or  which  gives  an 
article  an  appearance  better  than  it  properly  possesses  is,  of  course, 
illegitimate,  and  such  cases  are  not  here  considered.  Among  such 
uses  may  be  mentioned  that  of  color  in  pastry  to  impart  a  yellow 
color  thereto,  implying  the  presence  of  eggs,  when  they  are  either 
wholly  absent  or  are  not  present  in  sufficient  quantities  to  produce  a 
shade  of  color  which  would  indicate  a  superior  quality.  Such  color- 
ing is  frequently  resorted  to  in  macaroni,  spaghetti,  noodles,  and  the 
like,  and  it  has  also  been  stated  in  the  literature  that  such  coloring 
has  the  additional  function  of  concealing  dirt  actually  present  in  the 
flour. 

The  addition  of  red  coloring  matter  to  meat  products  to  give  them 
an  appearance  of  freshness  which  they  do  not  of  themselves  poa 
the  addition  of  red  coloring  matter  t<>  strawberry,  raspberry,  and 
similar  jams,  jellies,  and  preserves,  to  give  them  a  color  indicative  of 
exceptional  quality,  even  though  they  may  contain  none  of  the  fruit 
\vh<»se  presence  is  intimated  by  the  label  on  the  product ;  the  injection 
of  red  coloring  matter  into  ordinary  oranges  to  give  them  the  appear- 
ance of  blood  oranges;  the  sprinkling  of  lemons  and  oranges  with 
green  coloring  matter  t<>  give  them  the  appearance  of  a  particular 

origin  or  of  a  particular  state  of  ripeness  when  such  origin  or  state  of 
ripeness   ifl   without    foundation   in   fact;   the  injection  of  red   coloring 

matter  into  watermelons  to  give  them  the  appearance  of  ripeness, 

which  ripeness  they  do  not  possess,  are  practices  met  more  or  less 
frequently. 
Among  the  purposes  For  which  food  colors  are  said  to  he  used  and 

the  foods  BO  colored,  the  following  are  mentioned  in  the  literature: 

In  European  emu,' 

1.  Macaroni  ii  colored  \\ ith  Dinitrocn 
and  Martiui  V-  Hon  .  Handb  i 

2.  Cordials  and  liqueurs  with  Dinitroci  Arch.  Pkarm.,  < 


24  COAL-TAR  COLOKS  USED  IN  FOOD  PRODUCTS. 

3.  Oranges:  Biebrich  Scarlet  (163)  (Weyl,  Handbuch). 

4.  Pastry:  Dinitrocresol  (2)  (Weyl,  Handbuch). 

5.  Butter:  Dinitrocresol  (2)  (Weyl,  Handbuch). 

6.  To  whiten  flour:  Anilin  blue  (457)  (Zts.  Nahr.  Genussm.,  1906,  v.  12,  p.  298). 

7.  Noodles  are  colored  to  cover  up  cigar  butts,  burnt  matches,  mineral  oil,  etc. 
(Zts.  Nahr.  Genussm.,  Vol.  II,  p.  1018). 

In  the  United  States. 

8.  Jellies,  fruit  sirups,  soda  sirups,  jams,  ketchup,  cheap  cordials,  lemon  extract, 
milk,  butter,  cheese,  ice  cream,  confectionery,  pastries,  flavoring  extracts,  mustard. 
cayenne  pepper,  sausage,  noodles,  wines,  and  liqueurs  (Winton,  Connecticut  Agricul- 
tural Experiment  Station  Report,  1901,  pp.  179-182). 

9.  Cattle  feed  is  colored  yellow  (Gudeman,  J.  Amer.  Chem.  Soc,  1908,  v.  30,  p.  1623). 

10.  "Egg  color"  (399);  ''Macaroni  color"  (94);  "Tomato  catsup  color"  (105); 
"Raspberry  color"  (103);  "Mustard  color"  and  "Pie  filling  color"  (4);  "Orange 
color"  (87),  and  "Strawberry  red  color"  (55)  are  corresponding  United  States  com- 
mercial food  color  names  and  their  corresponding  Green  Table  numbers  (Meyer,  J. 
Amer.  Chem.  Soc,  1907,  v.  29,  p.  895). 

Dr.  E.  Ludwig,  of  Vienna,  stated,  upon  the  authority  of  Dr. 
Schacherl,  at  the  International  Congress  of  Medicine  held  in  Budapest, 
in  August,  1909,  as  follows: 

The  rather  widely  distributed  practice  of  coloring  baker's  goods  yellow,  such  as 
cakes  and  the  like,  further  the  yellow  coloring  of  pastry,  macaroni,  noodles,  and  so 
forth,  has  as  its  function  the  representation  of  a  very  large  egg  content  in  them;  this 
coloring  has  been  made  very  convenient  because  there  are  in  commerce  colors  intended 
specifically  for  this  purpose  and  designated  "egg  substitute"  and  which  have  nothing 
whatever  in  common  with  egg  yolk. 

Marmalades  such  as  apricot,  raspberry,  and  currant  marmalades  are  frequently  found 
in  a  colored  condition  in  commerce;  in  this  case  the  purpose  of  the  coloring  is  frequently 
to  cover  up  adulteration;  the  adulteration  may  consist  in  an  admixture  of  a  cheap 
fruit  pulp,  particularly  apple  pulp,  or  in  an  addition  of  glucose  sirup.  Since  these 
admixtures  do  not  possess  the  color  of  the  marmalades  they  are  simply  helped  along 
by  the  aid  of  color. 

Old  fruit  sirups  are  toned  up  with  color  and  then  sold  as  fresh-6irup. 

Red  colored  fermentation  vinegar  and  red  colored  vinegar  essence  as  well  as  vinegar 
made  from  such  essence  are  in  commerce;  such  coloring  has  for  its  purpose  to  represent 
the  product  as  "genuine  red  wine  vinegar,"  which  in  sonic  countries  is  highly  desired. 

So-called  "beer  color,"  said  to  be  an  extract  of  roast <<1  mall  (mall  caramel),  bin  fact 
nothing  but  ordinary  sugar  caramel  and  is  frequently  from  time  to  time  publicly  adver- 
tised; breweries  themselves  do  not  use  this  preparation,  but  it  has  been  frequently 
shown  that  in  small  taverns  by  means  of  this  color  local  beer  was  converted  into 
Bavarian  beer. 

Tin-  wholesale  coloring  oi  coffee  beans  serves  the  purpose  of  representing  a  better 
quality  than  it  actually  is. 

The  coloring  of  cocoa  and  chocolate  by  tin'  use  of  mineral  additions  and  also  of  coal- 
often  proven;  in  this  case  the  coloring  BGtVOI  exclusively  to  cover  up 

poor  quality,    in  the  case  of  good  products  such  coloring  is  not  practiced. 

I  olored  nusages,  and  in  fact  such  with  a  colored  meat  body  as  will  as  such  with  a 
colored  casing,  are  frequently  colored ;  coal-tar  colors  and  cochineal  serve  this  purj 
tin-  latter,  bowever,  only  for  the  meat    This  coloring  is  to  preserve  in  old  goods  the 
ranee  oi  if' 

Tin-  green  canned  goods  of  commerce  are  almost  all  colored  w  ith  copper  compounds. 


FOOD-COLOR  REQUIREMENTS.  25 

Tomato  pulp  frequently  comes  into  commerce  colored  with  a  coal-tar  color;  the  pur- 
pose of  such  coloring  is  to  impart  to  the  goods  the  appearance  of  having  been  prepared 
with  extraordinary  care.  In  all  these  cases  it  is  not  at  all  a  question  of  a  harmless 
change  of  the  natural  condition  of  the  food  product,  but  of  improper  manipulations 
which  are  adapted  to  deceive  the  purchaser  as  to  the  real  value  of  the  goods;  even, 
indeed,  to  mask  the  danger  to  health. 

III.  FOOD-COLOR  REQUIREMENTS. 
ADAPTABILITY  FOR  SPECIAL  PURPOSES. 

Not  all  coal-tar  colors  are  adapted  for  use  in  food  products. 
Colors  are  the  more  desirable  for  this  purpose  the  higher  their  tinc- 
torial power,  and  the  greater  the  resistance  they  offer  to  the  action 
of  the  materials  with  which  they  are  to  be  used,  and  under  the  con- 
ditions existing.  Obviously  only  such  colors  as  of  themselves  have 
their  tinctorial  properties  fully  developed  can  be  used,  and  all  such 
colors  as  require  a  mordant  to  develop  or  bring  out  the  color  are  not 
fit  for  nor  capable  of  use  in  food  products. 

Further,  if  the  colored  material  is  subjected  to  varying  tempera- 
tures in  the  process  of  manufacturing  foods,  it  should  be  able  to 
withstand  the  effects  of  such  temperatures,  as,  for  example,  in  the 
manufacture  of  candies.  The  colors  should  also  withstand  the  action 
of  reducing  agents,  such  as  are  generated  in  the  course  of  fermenta- 
tion and  decomposition  of  the  food  product,  or  where  a  preservative 
such  as  sulphur  dioxid  is  added  to  the  food  product  to  minimize  the 
effect  of  decomposition  of  the  food  upon  the  color.  Such  colors  arc 
put  on  the  European  market,  and  perhaps,  but  not  necessarily, 
on  the  United  States  market  with  preservatives  added  to  them. 
Most  of  the  coal-tar  colors  are  susceptible  to  the  action  of  sulphur 
dioxid,  particularly  when  the  latter  has  been  used  in  the  decolor- 
izing of  irhico^e,  and  Uranin  (510)  is  one  of  the  colors  found  to  have 
the  greatest  resistance  to  the  sulphur  dioxid  which  may  remain 
combined  in  candy. 

For  example,  the  book  entitled  "Henley's  Twentieth  Century 
Book  of  Receipts,  Formulas  and  IV  ."  published  in  1907,  on 

;'  sausage  color: 

h  i-  absolutely  necessary  in  using  aniline  colon  t-«  add  a  disinfectant  t<>  the  dye- 
itufl  solution,  tin-  <>l»jc<i  oi  which  is,  in  case  th<-  sausage  should  commence  to  d< 
toprevenl  decomposition  of  azo-dyestufi  by  the  (li.<niLraLr»'<l  hydrogen.     1: 
iracic  acid,  formaline  may  be  used  as  a  disinfectant. 

J.  Fraenkel  (Arbeit,  Kaiterl.  Gtsundh.  1902 }  p.  is,  j>j,.  r,is  521; 
abst.  '/J*.  Nahr.  OeMum^  I  16)  report-  a-  follow-  on 

the  composition   of  colors   used    in   coloring  sausages,  meat-,  and 
presen  es: 

l.  Blood  color:  Moisture,  r>  per  cent;  common  -alt,  6.6  per  cent;  boras,  H  per 
cent;  and  Ponceau  2B   G 


26  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

2.  Blood  red  for  meat  juices:  Liquid  of  a  specific  gravity  of  1.0163  not  affected  by 
acids  or  alkalis  and  containing  27  per  cent  total  solids;  of  these  total  solids  31  per  cent 
were  salt,  12  per  cent  borax,  and  the  remainder  Ponceau  2  R  (G.  T.  55). 

3.  Casing  red:  This  powder  contained  Orange  II  (G.  T.  86). 

4.  Sausage  red:  A  liquid  containing  Eosin. 

5.  Lobster  color:  A  liquid  of  specific  gravity  1.0064  containing  1.64  per  cent  of 
solids,  of  which  10.9  per  cent  were  salt  and  the  remainder  Ponceau  R  T  (G.  T.  44). 

G.  Possetto  (Zts.  Ndhr.  Unters.  Hygiene  }Yaarerik.  1891,  v.  5, 
p.  105)  cited  the  following  15  colors  as  being  used  for  the  coloring 
of  pastry : 

G.T.No.  G.T.No. 

Martius  Yellow 3     Tropseolin  00 88 


Tropseolin  000  No.  1 85 

Tropseolin  000  No.  2 86 

17 
Chrysoidin . 


18 
41 
Azoflavin 92 


Victoria  Yellow 2 

Naphthol  Yellow  S 4 

Aurantia  Yellow 6 

Acid  Yellow  G 8 

Acid  Yellow  R 9 

Citronin 91 

Tropseolin  0 84 

Algerian  Saffron  (a  mixture  of  Nos.  4  and  86  and  crocein). 
Prussian  Saffron  (composition  not  given). 

"Blood-red"  on  the  American  market  is  starch  colored  with  red  coal-tar  colors 
{Ibid.,  1896,  v.  10,  p.  114). 

"Butter  yellow"  is  a  clear  saponifiable  oil  of  reddish-yellow  color,  containing 
3  per  cent  of  anilin-azo-dimethylanilin  (No.  16  of  the  Green  Tables). 

PROPORTION  OF  COAL-TAR  COLOR  USED. 

The  amount  or  proportion  of  coal-tar  color  used  has  been  variously 
stated.  On  page  IV  of  the  Leffmann  translation  of  Weyl's  book 
entitled  "The  Sanitary  Relations  of  the  Coal-Tar  Colors,"  it  is 
stated  that  1  ounce  of  Auramin  (G.  T.  425)  will  color  2,000  pounds 
of  confectionery,  which  means  1  part  of  color  in  32,000  parts  of 
colored  product. 

Frentzel  (Zts.  Nahr.  Genussm.,  1901,  v.  4,  pp*  968-974),  on  author- 
ity not  given,  says  that  for  sirups  1  part  of  color  is  used  to  from 
4,000  to  5,000  parts  of  sirup;  in  colored  sugars  1  part  of  coloring 
inatter  to  from  1,333  to  4,000  parts  of  sugar;  and  in  flour  1  part  of 
coloring  matter  bo  from  666  to  1,000  parts  of  flour. 

In  pastry  1  to  100,000  parts  (Zts.  Nahr.  Unters.  Hygiene,  }\aarenli. 
1893,  v.  7,  p.  84). 

In  chapter  VII  (p.  47),  sections  L5,  16,  17,  and  is,  are  brought 
together  statements  made  before  the  commission  on  regulations  for 

the  Federal  food  and  drugs  act,  as  to  the  amount  of  color  contained 

in  colored  food  products.  Briefly  these  ate  as  follows:  Confec- 
tionery, l  pari  of  color  in  3,500  parts  of  product;  beverages  1  part 
of  color  in  128,000  parts,  256,000  parts,  1,024,000  parts;  butter,  420 
grains  of  color  to  1,000  pounds  of  butter;  or  1  part  of  color  to 
16,666  parts  of  butter. 


FOOD-COLOR   REQUIREMENT*. 


27 


One  ounce  of  color  to  30  pounds  of  "colored  food;"  the  colored 
food  was  not  further  defined:  which  means  1  part  of  color  in  480 
parts  of  colored  product. 

It  has  further  been  represented  that  1  part  of  color  is  sufficient 
to  whiten  250,000  parts  of  yellow  sugar. 

From  time  to  time  others  have  presented  information  as  to  the 
amount  of  color  used  in  food  products.  All  of  these  data  available 
have  been  tabulated,  showing  the  number  of  parts  of  colored  product 
containing  1  part  of  coal-tar  color,  arranged  in  the  order  of  the 
amounts  present : 


Food  ! 

Do  2 

Flour 

Do 

Sugar 

Confectionery. 

Sirups 

Sugar 

Sirups 

Confectionery. 

Butter 

Confectionery. 


100 

4S0 

666 

1,000 

1,333 

3,500 

4,000 

4,000 

5,000 

12,800 

16,  666 

20,000 


Contectionery 

Do 

Do 

Be  vera 


24, 576 

30. 000 



B0, 000 

Pastry 100.000 

Beverages 120, 000 

Do! 128 

Confectionery LS 

Whitening  sugar 250,  000 

Beverages 256. 000 

Do 1.024,000 


Grouped   according   to   the   kind   of   material   colored,    the   rai 
Lrivcn  arc  as  follows: 


Be \< tragi « 80, 000 ; 

120,000;  128.000;  I 

O(M);   l.HLM,000    l 

Biitt.-r b 

Confectionery 3,500; 

12,  800;  20, 000; 

:»J;30,000;  ' 
32,000;  192,000  j 

Flour 

1,000 


Food '  100; 

Pastry 100,000 

Sugar 1,333; 

-1.000 

Sirups i.ooi); 

5,000 
Whitening  sugar 25 


These  statements  have  emanated  From  persons  presumably  ac- 
quainted with  the  facts  of  their  own  practice,  and  if  that  presumption 
rrecl  it  appears  that  there  are  wide  variations  in  practice  not 

only  anions  individual  users,  lull  for  individual  colors.  No  attempt 
has  been  made  to  prove  or  disprove  these  statements  l»y  actual  deter- 
mination <'f  the  amount  of  color  contained  in  commercial  colored 
food  product-. 

The  s<>  chemical  individuals  on  this  market   for  food-Coloring  pnr- 

.  it  can  l»e  fairly  assumed,  have  been  tested  and  tried  out  . 
their  utility .  and  in  this  respect  further  tests  were  regarded  a-  super- 
fluous and  therefore  have  not  been  undertaken. 


1  Kind  not  <l.iiniirl . 


.  •>>  be  for  prtwrved  tomatoes. 


28  COAL-TAR  COLORS   USED   IX   FOOD  PRODUCTS. 

SUITABILITY  OF  SHADES  OF  PERMITTED  COLORS  AND  MIXTURES 

OF  SAME. 

The  shades  produced  by  the  seven  permitted  colors  are,  respec- 
tively, yellow,  orange,  blue,  green,  red,  bluish  scarlet,  and  brilliant 
cherry  red.  As  statements  are  found  in  the  literature  against  the 
use  of  all  of  the  chemical  individuals  producing  a  brown  or  a  violet 
shade,  it  will  be  necessary  to  produce  these  shades  by  a  proper  com- 
bination of  two  or  more  of  the  permitted  colors.  So  far  no  criti- 
cism with  regard  to  the  shades  produced  by  the  seven  colors  them- 
selves and  by  their  appropriate  mixture  has  been  made  that  has  been 
substantiated. 

Objection  has  been  made  to  the  violet  producible  from  blue  ami 
red,  on  the  ground  that  when  applied  to  a  food  product,  such  as 
candy,  the  component  parts  do  not  evenly  fix  themselves  upon  the 
material.  This  objection,  however,  has  not  been  pressed  and  proba- 
bly is  not  well  taken,  because  of  the  fact,  frequently  reported,  that 
few,  if  any,  coal-tar  colors  are  used  without  admixture  of  one  or  more 
other  colors  to  shade  or  to  tone  the  original  color.  Tins  criticism, 
therefore,  of  the  use  of  mixed  colors  can  be  regarded  as  not  a  serious 
objection. 

One  criticism  urged  with  considerable  persistency  against  the  seven 
permitted  colors  was  that  none  of  them  would  withstand  the  action 
of  the  organic  acids  ordinarily  found  in  beverages  such  as  lemonade, 
and  it  was  suggested  that  no  color  was  proper  for  use  for  such  pur- 
poses which  would  not  withstand,  unaltered,  for  a  period  of  12  hours 
the  action  of  a  10  per  cent  solution  of  citric  acid.  In  urging  tins 
objection  substitutes  were  suggested  for  the  permitted  colors.  The 
substitutes  so  urged  were  Tartrazin  (94),  Azorubin  (103),  Orange 
II  (86),  Ponceau  4  GB  (13),  and  one  other  color  designated  as  Scarlet 
SR,  of  whose  chemical  composition  no  information  whatever  was 
forthcoming.  (The  numbersin  parentheses  referto  the  Green  Tables.) 
Of  the  five  colors  suggested  it  can  be  said  that  concerning  all  but  No. 
103  adverse  statements  are  found  in  the  literature,  and  X<>.  86  is  spe- 
cifically regarded  by  every  observer  but  one  as  being  thoroughly 
poisonous.  The  suggested  substitute  list  is,  therefore,  objectionable 
on  the  ground  <>r  Lnjuriousness  to  health. 

To  best   the  validity  of  the  assertion  that,  none  of  the  permitted 

colors  could  withstand  the  action  of  citric  acid,  solutions  of  the  sug- 
gested colors,  as  well  as  of  the  permitted  colors,  each  one  in  a  thou- 
sand, were  submit  ted  to  the  action  of  citric  acid,  added  in  BUOh  quan- 
tity that  it  amounted  to  io  per  cent  of  the  total  bulk  of  solution. 
This  experiment  showed  that  Tartrazin  is  reddened  by  citric  acid, 
w  hereas  Naphtho]  Yellow  S  loses  in  tinctorial  power  to  a  slight  extent. 
The  shade  produced  l>y  Ponceau  4GB  can  bo  closely  imitated  by  a 
mixture  of  Naphtho]  Yellow  S,  Orange  J,  and  Amaranth,  all  per- 


FOOD-COLOR  REQUIREMENTS.  29 

mitted  colors.  There  is  no  choice  whatever  in  the  shade  produced 
by  the  desired  Azorubin  and  the  permitted  Amaranth,  nor  is  there 
any  difference  in  behavior  toward  citric  acid.  The  difference  in  the 
shade  between  the  desired  Orange  II  and  the  permitted  Orange  I  is 
so  small  that  it  requires  a  side-by-side  comparison  to  distinguish 
between  them.  Moreover,  the  desired  Orange  II  produces  a  precipi- 
tate when  brought  in  contact  with  the  citric  acid,  whereas  the  per- 
mitted Orange  I  does  not  so  precipitate.  The  permitted  Erythrosin 
is,  of  course,  completely  precipitated  by  the  citric  acid.  The  per- 
mitted Light  Green  and  Indigo  disulphoacid  are  weakened  in  tinctorial 
power  by  the  addition  of  the  citric  acid.  Of  these  colors  the  only 
ones  used  to  any  extent  in  beverages,  so  far  as  either  the  suggested 
or  permitted  list  is  concerned,  are  red,  yellow,  green,  and  orange. 

As  has  been  shown  the  permitted  reds  equal  the  desired  reds  and 
the  permitted  orange  is  better  than  the  desired  orange.  The  tinc- 
torial power  of  the  permitted  yellow  is  not  so  great  as  the  tinctorial 
power  of  the  desired  yellow,  but  this  difference  is  so  slight  that  the 
objection  urged  against  the  list  of  permitted  colors,  namely  that  they 
were  so  poor  in  quality  that  they  had  destroyed  a  profitable  and 
lucrative  business  in  the  coloring  of  beverages,  is  untenable  in  view 
of  the  fact  that,  assuming  a  price  of  $1  per  pound  for  Tartrazin,  and 
40  cents  for  Naphthol  Yellow  S,  and  using  them  in  the  proportions 
necessary  to  produce  a  lemonade  color  in  a  10  per  cenl  citric  acid 
solution,  it  would  take  5,000  quarts  of  finished  lemonade  to  cause 
an  increase  of  1  cent  in  the  cost  of  the  production  of  the  colored 
food  product;  that  is,  it.  increases  the  price  per  quart  by  one 
five-thousandth  of  a  cent. 

It  has  also  been  urged  that  the  permitted  green  is  not  good  enough 
for  cordials  and  liqueurs,  and  that  it  is  impossible  to  bring  about  the 
proper  green  by  the  use  of  the  permit  ted  yellow  and  blue.     This  criti- 
cism, however,  has  not  been  persisted  in;  the  fact  is  that  mixtur 
the  permitted  yellow  and  blue  can  be  made  so  as  to  obtain  any  desired 

shade  of  green,   having  a   \ellow  or  blue  Cast,   and  great   clarity  and 

brilliancy.     How  these  mixed  colors  would  look  after  a  long  period 

of  time  has  not    been  a-cert  allied. 

It  has  also  been  said  that  the  permitted  red,  Amaranth,  is  not  a 
color  suitable  for  I  he  coloring  of  st  raw  berry  jams  and  it  has  been  urged 

that    the  same  ehemieal   individual   under  another  eommereial   name 

is  better  than  the  permitted  red.    This  criticism  has  not  been  pressed, 

probably  for  the  reason  that,  it  can  not  he  substantiated. 

\  am  it  was  Claimed  that  the  deposits  to  he  noticed  in  bottled 
Lemonades  Were  due  to  Naphthol  Yellow  S,  hut  Solutions  of  Naphthol 
Yellow   S  in  citric  acid  have  remained  without   deposit   for  upward  of 

i;>  months;  if  is  possible  that  such  precipitation,  if  observed,  may  he 

due  to  an   admixture  of  the  nolipermit  t  ed  Orange    11    with   Naphthol 


30  COAL-TAB  COLORS  USED  IX  FOOD  PBODUCTS. 

Yellow  S,  and  this  difficulty  can  be  obviated  by  the  use  of  the  per- 
mitted Orange  I,  which  does  not  precipitate  in  the  citric  acid,  as 
shown. 

Xaphthol  Yellow  S  has  been  objected  to  on  account  of  the  bitter 
taste  it  is  said  to  impart  to  the  beverages  to  which  it  is  added,  and 
steps  have  finally  been  taken  by  those  interested  to  have  another 
yellow  placed  on  the  permitted  list. 

It  has  also  been  objected  that  the  permitted  bhie  is  not  suitable  for 
the  coloring  of  sugar,  first,  because  it  is  soluble,  and  second,  because 
of  the  unsatisfactory  shade.  It  may  be  sufficient,  in  answer  to  this 
criticism,  to  state  that  there  was  no  insoluble  blue  offered  on  this 
market,  and  there  was  no  blue  other  than  the  one  permitted  offered 
against  which  adverse  statements  did  not  exist  in  the  literature,  and 
in  view  of  this  state  of  affairs  the  criticism  may  be  said  to  be  not  well 
taken. 

As  against  all  these  specific  criticisms  it  has  been  repeatedly  stated 
by  those  in  a  position  to  know  that  they  have  found  no  difficulty 
whatever,  by  suitable  mixtures  of  permitted  colors,  in  reproducing 
any  desired  shade  of  any  desired  quality,  not  even  excepting  browns 
and  violets. 

Considering  all  of  these  criticisms,  therefore,  the  conclusion  seems 
reasonable  that  there  is  no  serious  or  permanent  objection  to  be  made 
against  the  seven  colors  selected,  either  as  to  qualities  for  food- 
coloring  purposes  or  range  of  producible  shades. 

IV.  CONFORMITY  OF  FOOD-COLOR  MARKET,  1907,  TO  RECOM- 
MENDATIONS OF  THE  NATIONAL  CONFECTIONERS'  ASSOCIA- 
TION, 1899.1 

Having  thus  shown  that  the  food-color  market  of  the  United  States 
contains  not  less  than  80  coal-tar  colors  which  are  distinct  chemical 
individuals,  of  which  74  are  entered  in  the  Green  Tables  and  6  are 
not,  the  next  question  to  be  considered  is  whether  all  of  these  sub- 
stances arc  harmless  and  fit  for  use  in  food  products. 

As  a  guide  in  determining  this  point  the  "Official  circular  from  the 
executive  committee  of  the  National  Confectioners'  Association  of  the 
United  St  at  es,"  pertaining  to  colors  in  confectionery,  dal  ed  February  1 . 
1899,  may  well  be  considered. 

The  function  of  this  circular  is  said  to  be  "to  throw  light  upon  the 
vexed  question  of  what  colors  may  be  safely  used  in  confectionery," 
evidently  because  "there  may  at  times  be  a  doubt  in  the  mind  of  the 
honest  confectioner  as  t<>  which  colors,  flavors,  or  ingredients  he  may 
safely  use  and  which  be  may  reject." 

The  circular  also  states  that  "but  infinitesimal  amounts  of  color 
(coal-tar  colors)  need  be  or  can  be  \\^^\  to  give  the  desired  effects," 

1  See  nlso  p.  45. 


FOOD-COLOR  REQUIREMENTS.  31 

and  in  view  of  this  statement  as  to  quantity  it  must  be  self-evident 
that  a  color  harmful  when  used  in  the  small  quantities  said  to  be  used 
in  confectionery  is  certainly  harmful  when  used  in  the  large  quantities 
used  in  coloring  other  food  products.  This  circular  under  the  head- 
ing, "Colors  that  are  injurious  and  therefore  to  be  rejected — Harm- 
ful organic  colors/'  enumerates  21  coal-tar  colors.  Of  these  21  colors, 
13,  or  61.9  per  cent,  were  among  those  submitted,  and  whose  com- 
position was  stated  by  reference  to  Green  Table  numbers;  the  Green 
Table  numbers  of  these  colors,  together  with  the  number  of  sources 
from  which  they  were  obtained,  follow: 

Green  Number         Green  Number 

Table  of  Table  of 

numbers.  sources,      numbers.  sources. 

11 2     169 1 

17 2     197 4 

18 1     201 2 

84 2     398 2 

86 8  I  584 1 

95 2  I  650 2 

106 5  I 

Out  of  these  13  colors  3  each  came  from  one  source;  7  each  came 
from  two  sources;  1  came  from  four  sources;  1  came  from  five 
sources,  and  1  came  from  eight  sources,  out  of  a  possible  12;  that  is, 
one  was  wanted  by  more  than  half  the  sources. 

It  is  further  to  be  noted  that  of  the  trade  names  given  to  the  sub- 
mitted products  of  Class  I  the  following  appeared  among  the  harmful 
list  of  this  circular  and  also  were  found  in  identical  form  and  spelling 
on  the  labels  of  the  submitted  products: 


1.  Bismarck  Brown. 

2.  Chrysoidin  R. 

3.  Chrysoidin  Y. 

1.  Mandarin  ( i  extra. 

5.  Naphthol  Green  B. 

6.  Napthol  Yellow. 

7.  New  Coccine. 


8.  Orange  A. 

9.  Orange  A  extra. 

10.  Orange  G. 

11.  Orange  II. 

12.  Scarlet. 

L3.  Veeuvin  B. 

14.  Croceio  Scarlet  5  B. 


The  following  parallel  will  serve  to  show  the  great  resemblance 
between  the  names  given  to  the  harmful  colors  of  the  circular  and 
those  found  on  the  Bamples  submitted: 

(  irruhir's  }hu infnl  I'tsl .  Labi  It  af  suhmittt  <l  samj>l<  s. 

Methylene  Blue  B  B Methylene  Blue  B. 

Methylene  Blue  B  B  crystal* Methylene  Blue  D. 

Methylene  Blue  B  BG Methylene  BlueO 

Methylene  Blue  D  B  B 

New  Coccine New  I  0  Z. 

\«\V  ('..<(  in.  ■  z. 

Naphthol  Green  B Naphthol  Green. 


32  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

Circular's  harmful  list.  Labels  of  submitted  samples. 

Orange  II Orange  II  Z. 

Victoria  Yellow Victoria  Yellow  Cone .  Z . 

Victoria  Yellow  Cone.  T  Z. 

Acid  Yellow Acid  Yellow  G. 

Bismarck  Brown  G Bismarck  Brown  B. 

Bismarck  Brown  T Bismarck  Brown  B  216. 

Bismarck  Brown  Dark. 

Bismarck  Brown  R  X. 

Bismarck  Brown  T  D. 

Bismarck  Brown  Y  Bril. 

Bismarck  Brown  Y  Dark. 

Bismarck  Brown  2  R  X. 
Chrysoin Chrysoin  Brown  G  Z. 

Chrysoin  G  E  Z. 

Chrysoin  R  E  Z. 

Chrysoin  R  Z. 

Cochineal  Red  A Cochineal  Red. 

Crocein  Scarlet  3  B Crocein  Scarlet  10  B. 

Crocein  Scarlet  7  B 

Crocein  Scarlet  8  B 

Fast  Brown  G Fast  Brown  N. 

Fast  Brown  0. 
Fast  Yellow Fast  Yellow  G. 

Fast  Yellow  0  3  3. 

Fast  Yellow  0  3  4. 

Fast  Yellow  Y. 

Imperial  Scarlet,  in  powder,  extra Imperial  Scarlet  3  B. 

Safranin Safranin  S  P. 

Safranin  A  G  extra. 
Safranin  AGT  extra. 
Safranin  Cone. 
Safranin  extra  G. 
Safranin  FF  extra  No.  0. 
Safranin  G  extra  GGS. 
Safranin  G  000. 
Safranin  T. 

This  comparison  disclosed  a  considerable  lack  of  conformity  be- 
tween the  United  States  food-color  trade  in  1907  and  the  circular  of 
February,  1899,  upon  whose  preparation  for  seven  months  prior  to 
its  date  "a  great  deal  of  thought  and  labor  have  been  given  to  a 
thorough  investigation  of  the  whole  subject  of  'colors  in  confec- 
tionery,' in  which  the  committee  lias  been  hugely  aided  by  the 
researches  of  the  association's  chemist  and  by  the  results  of  his 
analytical   tots"   and   whose  "classifications   have  been  carefully 

made,  and  are  based  upon  the  authority  of  the  eminent  chemists, 
Prof.  Ivocuig  ami  Prof.  Wcvl,  upon  the  resolutions  of  the  Swiss 
chemists  and  upon  the  French  ordinances  regarding  the  coloring  of 
food  products,"  and  which  list  was  expected  to  be  ''of  value  to  color 


FOOD-COLOR   MARKET,   1907. 


33 


dealers  and  chemists/'  and  also  was  published  to  assist  the  confec- 
tioner in  obeying  "the  letter  and  the  spirit"  of  the  pure-candy  laws. 
Under  the  heading  "Colors  that  have  been  shown  to  be  harmless 
as  used  in  the  confectioner's  art,  harmless  organic  colors,"  this  cir- 
cular enumerates  36  colors,  for  4  of  which  there  are  no  Green  Table 
numbers.  Of  the  32  colors  having  Green  Table  numbers,  20,  or  62.5 
per  cent,  were  among  those  colors  submitted.  The  Green  Table  num- 
bers of  these  colors,  together  with  the  number  of  sources  from  which 
they  were  obtained,  follow: 


Green 

Table 

numbers. 


9. 

13. 

55. 

65. 

85. 
103. 
105. 
107. 


Number 

of 
sources. 

...  10 

5 

...  1 

...  6 

5 

...  2 

...  2 

...  6 

...  1 

...  7 


Green 

Table 

numbers. 

240 


269. 
287. 
427. 
448. 
451. 
462. 
512. 
517. 
520. 


Number 

of 
sources. 


Of  these  20  colors  5  each  came  from  1  source;  5  each  came  from  2 
sources;  1  came  from  3  sources;  1  came  from  4  sources;  4  each  came 
from  5  sources;  2  each  came  from  6  sources;  1  came  from  7  sources, 
and  1  came  from  10  sources;  that  is,  only  2  were  wanted  by  more 
than  half  the  makers  or  importers,  and  only  4  by  half  the  sources. 

It  will  be  noted  that  this  circular  provides  for  a  total  of  only  57 
different  coal-tar  colors;  the  number  of  avowed  colors  submitted 
reached  80,  or  23  in  excess  of  this  number,  and  further,  that  out  of 
the  57  colors  referred  to  in  t  his  circular  only  33  appeared  among  those 
colors  submitted  whose  composition  was  acknowledged,  ><»  that  for 
47,  or  58.8  ()<■!•  cent  of  the  avowed  submitted  colors,  t  his  circular  is  no 
specific  collide.  From  the  data  obtainable  from  this  circular,  the 
following  tabulation  can  be  made: 

Harmfukteu of  tubmitted colon  t><is'<l  <>n  list  in  circular. 


lot. 1. 

Total  en 

market. 

market. 

Ciroilur's 

Branding 

list. 

n  rata] .   . 

Frrcciit. 

I'rrcent. 

These  figures  disclose  a  considerable  and  self-evident  disregard  of  t  he 

request .  t  hen  eight  years  old,  as  made  l»y  t  he  National  <  'on feet  loners' 

97291  '     Hull,  l  ff     12  — 3 


34  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

Association  of  the  United  States,  that  coal-tar  colors  designated 
by  it  as  ' 'colors  that  are  injurious  and  therefore  to  be  rejected, 
harmful  organic  colors"  be  not  used  in  confectionery,  and  by  implica- 
tion that  they  should  not  be  used  in  other  food  products. 

In  view  of  this  disregard  with  respect  to  13  coal-tar  colors  out  of 
33  on  the  United  States  market  in  the  summer  of  1907,  dealt  with  in 
this  confectioners'  list,  the  conclusion  seemed  justified  that  the  action 
regarding  other  coal-tar  colors  on  the  United  States  market  in  the 
summer  of  1907  was  equally  heedless  or  indifferent,  a  conclusion 
which  is  borne  out  by  the  material  brought  together  under  section  IX. 

The  necessity  of  adhering  to  some  unequivocal  terminology,  as  has 
been  done  in  these  pages  by  referring  to  the  serial  numbers  in  the 
Green  Tables,  appears  from  the  following: 

Trade  names  are  not  definite  with  respect  to  the  composition  of 
the  article  sold  under  a  given  name,  although  tinctorially  the  colors 
may  be  substantially  equivalent.  In  the  Green  Tables  there  are  not 
less  than  29  instances  where  the  same  trade  name  is  applied  to  two 
or  more  different  chemical  individuals.  In  some  cases  these  chemical 
individuals  are  fairly  closely  related,  in  others  they  are  only  remotely 
related.  When  the  differences  are  greater  than  the  presence  or 
absence  of  a  sulpho  group  or  the  use  of  methyl  for  ethyl  or  the  reverse; 
the  instances  are  given  below: 

1.  Cotton  Yellow 128  Primulin-azo-m-pheriylene-diamin-disulphonicacid. 

191  Diphenylurea-riisazo-bi-salicylic  acid. 

2.  Methyl  Eosin 513  Methylated  tetrabromo-fluorescein. 

375  Dinitro  dibromo  fluorescein. 

3.  New  Yellow 88  p-sulphanilic  acid  azo-diphenylamin. 

91  Nitration  product  of  diphenylamin  yellow. 

4.  Orange  ITT 23  Meta-nitranilin  azo-R  salt. 

87  p-sulphanilic  acid  azo-dimethylanilin. 

5.  Orange  X 43  Toluidin  azo-Schaffer  acid. 

88  p-sulphanilic  acid  azo-diphenylamin. 

6.  Orange  R 97  o-toluidin-monosulphoiiic  acid  azo-hetanaphthol. 

15  Anilin-azo-R  salt. 

99  Xylidin  sulphoacid-azo-hetanaphthol. 

7.  Toluylene  Red 201  Dichloro-benzidin  disazo  R  salt. 

580  Dimethyl  diamido  toluphena/.in. 

The  following  quotation  also  bears  on  this  point : 

In  attempts  i"  group  the  aniline  colors  a  kind  of  uncertainty  appears  even  among 
color  chemi  -i  .  The  same  trade  name  docs  not  always  correspond  to  the  same  prepara- 
tion.   Many  preparations  are  not  chemical  individuals,  hut,  mixtures  of  related  colors. 

Many  preparations  an;  'standardized  "  for  the  trade;  for  example,  with  dextrin.  On 
account,  of  the  patent  laws,  factory  secrets  surround  the  produd  LOO  of  many  coloring 
matters,  and  frequently  Statements  are  mot.  with  which  are  directly  intended  inv  the 

purpose  of  mi  leading  competition,  (Ilueppc,  Die  Methodcn  dcr  BaHcricnforschung, 
5th  cd.,  1891,  p.  105.) 


LEGAL  ENACTMENTS.  35 

V.  SOME  LEGAL  ENACTMENTS  RELATIVE  TO  THE  USE  OF 
COAL-TAR  DYES. 

LIST  OF  THIRTEEN  FOREIGN  LEGAL  ENACTMENTS. 

The  13  foreign  legal  enactments  compared  are  as  follows: 

1.  The  Austrian  regulation  of  March  1,  1886,  which  forbids  Xo. 
483  of  the  Green  Tables  and  all  anilin  colors. 

2.  The  law  of  Austria  of  May  1,  1886,  which  forbids  Xo.  1  of  the 
Green  Tables  and  all  anilin  colors. 

3.  The  Austrian  regulation  of  September  19,  1895,  in  which  cer- 
tain colors  only  are  permitted,  and  all  others  are  forbidden.  There 
are  16  titles  of  permitted  colors  in  this  law,  but  these  are  in  some 
cases  so  elastic  and  so  indefinite  as  to  include  47  entries  in  the  Green 
Tables. 

4.  The  Austrian  law  of  January  22,  1896,  in  which  there  are  17 
titles,  but  these  are  sufficiently  elastic  to  allow  of  22  entries  in  the 
Green  Tables  being  included  in  them. 

5.  The  German  law  of  July  5,  1887,  which  specifically  prohibits 
only  Xos.  1  and  483  of  the  Green  Tables.  The  interpretation  which 
seems  to  be  generally  placed  upon  this  law  is  that  all  other  Green 
Table  members  are  permitted  in  Germany  for  use  in  foods. 

6.  The  Italian  law  of  February  7,  1892,  forbidding  all  colors  except 
9  different  titles,  which,  however,  were  elastic  enough  to  include  32 
entries  in  the  Green  Tables. 

7.  The  law  of  Italy  of  February  7,  1902,  which  prohibits  .17  entries 
in  the  Green  Tables,  and  permits  11  specifically. 

8.  The  Italian  decree  of  June  29,  1893,  in  which  there  were  7 
titles  of  permitted  colors  sufficiently  elastic  to  include  34  different 
individuals. 

9.  The  Italian  decree  of  March  24,  1895,  forbidding  four  titles  cov- 
ering only  four  entries  in  the  Green  Tables. 

10.  The  French  police  ordinance  of  May  21,  1885,  in  which  is1' 
entries  in  the  Green  Tables  were  prohibited. 

11.  The  French  police  ordinance  of  December  31,  1890,  in  which 
469  entries  of  the  Green  Tables  were  prohibited,  and  which  also 
permitted  under  9  titles  23  entries  in  the  Green  Tables. 

12.  The  Belgian  law  of  1891,  which  specifically  forbids  only  four 
entries  in  the  Green  Tables. 

I."!.    The  law  of  (he  Canton  of  Te»in,  dated    May    Is,    iso;.   which 

forbids  only  -1  specific  entries  in  the  Green  Tables. 

SUMMARY  OF  COLORS  PERMITTED  BY  THESE  LEGAL  ENACTMENTS. 
An  examination  of  the   13  legal  enactments  made  in   Knrope  with 

respect  to  the  use  of  coal-tar  colors  in  food  products  discloses  consid- 
erable difference  of  opinion  as  to  the  barmfulness  or  the  harmlessnesfl 
of  even  the  same  chemical  individuals.    To  prepare  an  approximate 


36 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


and  comprehensive  summary  of  the  effect  of  such  legislation,  the 
following  plan  has  been  followed : 

The  provisions  of  a  selected  number  of  laws  and  regulations,  13  in 
number  and  dating  from  1883  to  1902,  were  read  with  respect  to 
permission  or  prohibition  of  the  695  chemical  individuals  listed  in  the 
Green  Tables.  The  effect  of  each  law  upon  each  separate  entry  in 
the  Green  Table  numbers  was  noted,  either  as  permitted,  forbidden, 
or  noncommittal  when  the  law  was  silent  upon  such  entry;  the  laws 
were  read  with  the  understanding  that  what  was  not  forbidden  was 
permitted,  and  what  was  neither  forbidden  nor  permitted  was  non- 
committal; if  this  were  an  incorrect  or  improper  procedure  the 
number  of  permitted  colors  would  be  reduced  but  not  augmented. 
For  the  purposes  of  this  first  approximation,  no  attempt  was  made 
to  segregate  those  specifically  permitted  from  those  permitted  by 
blanket  expressions  or  phrases. 

For  the  purposes  of  a  side-by-side  comparison,  the  term  "  index 
number1'  was  coined;  this  ''index  number"  gives  in  the  first  place  the 
number  of  legal  enactments  that  permit  the  color;  in  the  second  place 
the  number  of  enactments  that  forbid  it;  and  in  the  third  place  the 
number  of  enactments  that  are  silent  or  noncommittal.  Thus:  2S3 
as  an  index  number  would  mean  2  enactments  permit,  8  forbid, 
and  3  are  noncommittal;  so  that  an  index  number  with  the 
highest  hundreds  would  have  the  greatest  number  of  permissions, 
and  with  the  highest  tens  would  have  the  highest  number  of  pro- 
hibitions. With  this  understanding  of  these  terms,  the  following 
table  of  so-called  index  or  "P.  F.  N."  numbers  is  offered: 

Thirteen  legal  enactments  classified  by  Green  Table  numbers  and  the  "P.  F.  N.  figure," 

or  "index  number." 


Total 
number 
of  Green 

Table 
entiles. 

Index 

number. 

Qreen  Table  numbers. 

l 

1 

3 

217 

1 
366 

29 

3 
1 

7 
■J 
2 
3 
3 
11 

1 
ti 

2 

184 
J74 

2,10,1 
304 

373 

891 
468 

IM 

544 

663 

:»7i 
643 

661 

(.70 
71-' 
751 

081 

483. 

1-3. 

394-411,  416-426,  428-434.  |S5»,  436-446,  484-492,  528-661,  564-683,  688 

600.602-649,651-691,693-696. 
108. 

0,7, 10,11, 12,14, 10,19-22,35-40,42, 4:v«-V:>4,.r,S-04.  66-83,  89,  90.  88,  84,  86- 
101,104-106,  L09-113,  115  L45,  149,  L51-156.  168,  L69,  161,  162,  164-168, 
17_\  197.  1''  •                     1,412-414,493-611, 

(46,  1 1                                                               178,  179,  181, 

154,477,51  1,519,622. 
662,601. 
515,516. 
480,514 
44,11  i 

l  ',  L5  35,92,108,146  1  K 160, 160, 117. 
l,    L8  ii.  169,512,518. 
451,  162. 
4, 55. 54,57,102 

lis 

467. 
167,171. 

Italicized  Agorei  Indioate  colors  permitted  by  T.  T.  i>.  76, 


LEGAL  ENACTMENTS.  37 

From  the  table  it  appears  that  there  is  no  one  Green  Table  number 
that  is  permitted  by  each  and  all  of  these  13  legal  enactments,  nor 
is  there  any  one  color  that  is  prohibited  by  each  and  all  of  these  13 
legal  enactments;  and  as  late  as  1902  there  was  considerable  con 
fusion  as  to  what  should  or  should  not  be  permitted  or  forbidden. 
That  the  European  enactments  were  not  in  reality  consistent  or 
effective  appears  from  the  following: 

1.  In  respect  to  the  use  of  coal-tar  colors,  the  views  as  to  their  harmfulness  or  hann- 
lessness  are  very  divergent,  and  this  uncertainty  is  expressed  in  the  various  legislative 
enactments,     (v.  Raumer,  Zts.  Nahr.  Unters.  Hygiene  d'Waarenk.,  1895,  v.  9,  p.  207.) 

2.  After  eating  groats,  which  no  doubt  were  free  from  ordinary  poisons  but  had  been 
colored  with  Martius  Yellow,  a  whole  family  became  sick.  Since  this  coloring  matter 
is  not  mentioned  among  those  which,  under  the  law  of  July  5,  1S87,  are  forbidden 
for  the  purpose  of  coloring  articles  of  food,  a  complaint  could  not  be  lodged.  Never- 
theless, the  use  of  Martius  Yellow  for  the  coloring  of  articles  of  food  would  seem  to  be 
dangerous,  since  this  coloring  matter  exerts  poisonous  •  It  is  a  weakness  in 
the  law  that  coal-tar  colors,  of  which  new  members  arc  continuously  appearing  on 
the  market,  and  whose  physiological  action  is  unknown,  should  be  at  all  permitted 
for  the  coloring  of  articles  of  food.  (Dietrich,  Th.,  Jahresberichte  der  landwirthschoft- 
lichenVersuchsstation,  Marburg,  1900-1901,  p.  13;  abaft.  Zls.  Nahr.  Genustm.,  190£,  r.  5, 
p.  364.) 

On  account  of  their  large  number  and  the  great  diversity  of  opinion 
as  to  harmfulness  of  some  coal-tar  colors  and  the  harmlessness  of 
others  therein  reflected,  no  attempt  was  made  to  collect  all  the 
legal  enactments  and  regulations  made  with  respect  to  coal-tar 
dyes.     The  foregoing  are  typical  of  the  remainder. 

COLORS  SAID  TO  BE  PERMITTED  UNDER  THE  GERMAN  LAW 

OF  1887. 

That  some  of  the  laws  did  not  employ  specific  terms  but  used  those 
possessed  of  a  «;reat  degree  of  elasticity  appears  from  the  following 
t  aken  from  WeyPs  "Sanfl  ary  relat  i<>ns  of  \  lie  coal-tar  colors,"  page  38, 
concerning  the  Chamber  of  Commerce  and  Trade  of  Sonneberg  which 
declared  on  December  4,  1887,  that  the  German  law  of  July  .".  L887, 
allowed  the  unrestricted  use  of — 

All  blue  an<l  violet  anilin  (thai  ia  coal-tar)  colon,  all  ponceaus,  all  orange  colon, 
Methyl  Green,  Brilliant  Green,  Malachite  Green,  Chryeoidin,  Naphtho]  Yellow,  Man  i  us 
Yellow.  En  rin,  Phloxin,  Bafranin,  Erythrosin,  Fuchnn,  Phenylene  Brown,  and  Anilin 
Black. 

This  amounts  t<>  not  less  than  L'.;:;  permitted  colors,  as  will  now  be 
shown. 

Using  the  Green  Tables  as  a  guide  it   will  be  found  that   under  the 

above  ruling  there  are  to-daj  no  less  than  107  blue  coal-tar  colors 
which  could  be  wm><\  for  f<»«..l  coloring.     The}  are  arranged  as  follows, 

showing  the  comments  <<n  same  in  the  literature. 


38  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

BLUE    COLORS. 

Unfavorable:  478,  479,  488,  490,  572,  602,  639.     (Total,  7.) 

Favorable:  477,  599,  600,  692.     (Total,  4.) 

Contradictory:  287,  457,  480,  563,  601,  650,  689.     (Total,  7.) 

Not  reported  an:  36,  83,  119,  142,  175,  189,  209,  246,  247,  254,  257,  263,  266,  288,  290, 
291,  292,  293,  294,  295,  301,  302,  310,  311,  314,  315,  316,  317,  318,  319,  323,  327,  345, 
347,  348,  351,  352,  356,  359,  364,  430,  432,  439,  440,  442,  444,  456,  473,  476,  481,  482, 
487,  492,  509,  542,  551,  556,  558,  559,  560,  562,  569,  595,  598,  608,  611,  612,  615,  618, 
619,  621,  625,  627,  628,  634,  637,  638,  640,  641,  642,  643,  652,  655,  656,  657,  664,  682, 
693,  694.     (Total,  89.) 

Similarly  there  would  be  50  violets  which  are  classified  as  follows: 

VIOLET   COLORS. 

Unfavorable:  620,  649.     (Total,  2.) 

Favorable:  467,  593.     (Total,  2.) 

Contradictory:  450,  451.     (Total,  2.) 

Not  reported  on:  30,  34,  36,  118,  176,  179,  207,  244,  246,  248,  252,  256,  273,  320,  336, 
338,  340,  342,  343,  444,  452,  454,  455,  463,  464,  465,  466,  468,  469,  470,  471,  472,  474,  486, 
506,  507,  525,  552,  579,  581,  585,  592,  613,  625.     (Total,  44.) 

Similarly  there  would  be  18  ponceaus  which  are  classified  as  follows: 

PONCEAUS. 

Unfavorable:  None. 

Favorable:  169,  448.     (Total,  2.) 

Contradictory:  13,  15,  55,  160,  163.     (Total,  5.) 

Not  reported  on:  44,  56  \  571,  108,  113,  114,  146,  147,  148,  150,  165.    (Total,  11.) 

Similarly  there  would  be  35  Oranges  which  are  classified  as  follows: 

ORANGES. 

Unfavorable:  2,  97.     (Total,  2.) 
Favorable:  85.     (Total,  1.) 

Contradictory:  14,  18,  43,  86,  87,  88,  95.     (Total,  7.) 

Not  reported  on:  10,  23,  47,  54,  99,  100,  136,  162,  196,  217,  218,  222,  225,  235,  236, 
265,  275,  392,  406,  408,  409,  529,  531,  545,  547.     (Total,  25.) 

The  remaining  23  colors  named  are  classified  as  follows: 

MISCELLANEOUS. 

Unfavomhh:  Martius  Yellow  (3). a    (Total,  1.) 

Favorable:  Naphthol  Yellow  S.  (4);  Eoein  (512,  517,  521);  Phloxin  (521);  Erythrorin 

(517).     (Total,  6.) 

Contradictory:  Brilliant  Green  (428  ;  Malachite  Green  (427);  ChryBoidin  (17,  L8,  it  ; 

Sairanirj  (584)';  Fuchrin  (448);  Phenylene  Brown  (197).    (Total,  8.) 
Not  reported  on:  Methyl  Green  (460,  461);  Eoean  (51 1,  515);  Phloxin  (518);  Bafranin 

(583,  585);  Erythrosin  (516);  Anilin  Black  (577).    (Total,  9.) 

It  will  be  noticed  tli.it  names Buch  as  Eosin,  Erythrosin,  and  Phloxin 
appear  in  more  than  one  classification;  thus  sumo  of  each  arc  favor- 
ably reported  on  and  the  others  are  nol  reported  on  at  all. 


1  Nos.  5<-  Hid  67  in  Included  tmong  I  ii«'  permitted  colors  of  the  Austrian  lew, 
•The  number!  iu  paMntneni  following  the  names  are  the  Green  Table  numbers. 


LEGAL  ENACTMENTS. 


39 


The  233  colors  said  by  the  Sonneberg  Chamber  of  Commerce  and 
Trade  to  be  entitled  to  unrestricted  use  in  food  coloring  under  the 
German  law  of  1887  referred  to  may  also  be  classified  as  follows: 

Summary  of  classification  of  colors  permitted  under  the  German  law  of  1887  according  to 

comments  in  the  literature. 


Blues.. 
Violets. 


Ponceaus 

Oranges 

Miscellaneous. 


Total. 


Class. 


Total. 


107 
50 
18 
35 
23 


233 


Comments  in  the  literature. 


Unfa- 
vorable. 


Favor- 
able. 


Contra- 
dictory. 


29 


Not  re- 
ported 
on. 


178 


Out  of  these  233  colors  only  55,  or  about  one-fourth,  have  been 
reported  on  in  the  literature  and  the  remaining  three-fourths  have 
not  been  examined  at  all.  To  the  55  examined  and  reported  on 
there  may  be  added  2,  namely,  Xos.  56  and  57,  since  they  are  included 
among  the  colors  once  permitted  by  law  in  Austria,  thus  making  a 
total  of  57  examined  out  of  232.  Adding  these  two  to  the  14  favor- 
ably reported  on  makes  a  total  of  16.  It  finally  appears  that  11 
out  of  57  colors  examined  would  in  the  light  of  present  knowledge 
be  improper  to  be  used  in  food  and  12  at  least  should  not  be  used  for 
such  purposes  at  all. 

The  classification  into  unfavorable,  favorable,  contradictory,  and 
not  reported  on  is  based  upon  the  tabulation  on  "page  63;  if  that  is 
substantially  correct  the  above  conclusions  are  also  true. 

The  foregoing  side-by-side  comparison  of  13  legal  enactments, 
while  it  makes  no  claim  to  being  absolutely  and  wholly  accurate  in 
all  the  classifications  or  conclusions  drawn,  is  no  doubt  a  fair  reflec- 
tion of  the  condition  of  mind  of  those  framing  the  enactments,  and 
consequent  ly  of  information  upoE  which  t  boss  enact  ments  were  based; 
and  the  conclusion  would  therefore  seem  t<>  he  justified  that  the  fact 

that  a  color  has  been  permitted  or  has  been  forbidden  by  any  one  or 

the  majority  of  t hoe  Legal  enactments  ought  n.»t   t<»  constitute  a 

clean  bill  of  health,  n<»r  ;iu  indict  men t  .  a--  the  CaS6  may   he. 

This  side-by->ide  comparison  must   ii"t   he  pushed  t«-  extremes; 

indeed  the  extent  to  which  it  can  he  employed  LS  naturally  \«-ry  lim- 
ited, and  the  purpose  for  which  it  was  made  was  t<>  reflect  in  a  manner 

easily  and  comprehensively  grasped  the  confusion  and  inconsistencies 
which  very  persistently  force  themselves  upon  the  mind  of  a  person 

reading  those  enactments  and  haying  in  mind  the  chemical  individ- 
uals at  which  they  are  aimed. 


40  COAL-TAR   COLORS  USED   IN    FOOD   PRODUCTS. 

The  definite  lesson  to  be  learned  from  this  side-by-side  comparison 
is  that  these  enactments  in  many  cases  employed  terms  so  vague  and 
indefinite  as  to  permit  the  use  of  some  bad  colors  as  well  as  all  good 
ones,  that  is  they  were  not  sufficiently  definite  to  exclude  all  that 
were  harmful. 

DEFINITENESS    AND    DETAIL   NECESSARY   TO    EFFECT    QUALITY 

CONTROL. 

Tins  apparent  state  of  confusion  in  legal  enactments  that  pre- 
ceded the  summer  of  1907  was  a  very  strong  factor  in  the  formation 
of  the  conclusion  that  in  order  to  be  effective  any  law  or  regulation 
dealing  with  coal-tar  colors  for  use  in  foods  must  prohibit  every  coal- 
tar  color  except  certain  definite  specific  ones. 

The  Austrian  laws  of  September  19,  1895,  and  of  January  22,  1896, 
provided  for  quality  control  by  public  and  other  laboratories  of  the 
coal-tar  colors  put  upon  the  market  for  use  in  foods;  the  results  of 
such  control,  as  reported  in  the  Zeitschrift  fur  Nahrungsmittel- 
Untersuchung,  Hygiene  und  Waarenkunde,  1896,  v.  10,  p.  335,  are 
as  follows: 

Coloring  matters  of  commerce  are  mostly  mixtures  of  various  coloring  matters,  a 
right  which  manufacturers  will  not  part  with;  and  further,  while  it  is  indeed  possible 
to  test  the  coloring  matter  in  substance,  it  is  nevertheless  impossible  to  test  it  in  the 
very  small  amounts  which  are  used  in  the  coloring  of  foodstuffs  and  to  determine 
with  certainty  the  identity  of  the  color  as  to  whether  it  is  or  not  one  of  the  permitted 
colors. 

Of  21  samples  of  coloring  matter  examined,  14  were  objectionable,  partly 
because  of  false  labeling,  or  because  they  were  mixtures,  partly  because  they 
contained  poisonous  metals,  or  a  forbidden  coloring  matter.  Thus,  a  so-called  "Ever- 
green" was  Naphthol  Green  B,  a  poisonous  nitroso  color;  Malachite  Green  contained 
zinc;  an  Acid  Magenta  and  a  Rosalin  contained  traces  of  copper;  Ponceau,  Eosin, 
Brown,  and  Roccellin  contained  traces  of  tin;  Orange  I  and  Waterblue  contained 
traces  of  tin  and  zinc.  The  last-named  coloring  matters  were  therefore  not  pre] tared 
in  proper  state  of  purity. 

The  authorities  in  Vienna  examined  four  and  rejected  two  colors.  {Ibid.,  1S98, 
p.  107.) 

The  Swiss  authorities  exercised  control  over  colors,  after  they 
reached  the  market,  with  the  result  that  the  authorities  in  Basle 
examined  ten  colors  and  rejected  one.     (Ibid.,  1897,  p.  292.) 

These  facts,  together  with  the  knowledge  derived  by  even  the  most 
superficial  ocular  examination  of  the  294  specimens  received  in  the 
summer  of  1907,  played  a  very  great  part  in  the  formation  of  the  con- 
clusion thai  control  of  quality,  in  order  to  be  even  reasonably  effec- 
tive, must  be  thoroughgoing,  and  that  colors  must  be  excluded  from 
I  lie  market  until  they  prove  themselves  to  be  clean,  rather  than 
permitted  promiscuously  and  then  driven  out  of  the  market  by  the 
authorities  if  unsuitable. 

The  effective  quality  control  of  food  colors  requires  careful  and 
searching  examination  of  a  kind  which  can  not  usually  be  obtained 


LEGAL  ENACTMENTS.  41 

by  the  general  purchasing  public.  The  quality  of  the  food  colors 
offered  in  the  summer  of  1907  varied  greatly,  and  the  substances 
contaminating  them  were  of  such  indefinite  and  probably  variable 
composition  (of  whose  physiological  action  nothing  definite  was 
known  and  whose  quick  and  certain  detection  in  the  colored  food 
product  would  be  very  complicated,  if  not  impossible)  that  quality 
control  of  greater  efficiency  than  that  exercised  by  those  selling 
food  colors  in  the  summer  of  1907  seemed  necessary  on  the  part  of 
the  authorities  having  charge  of  the  enforcement  of  the  food  and 
drugs  act. 

The  points  of  original  entry  of  food  colors  into  the  United  States 
food-color  market  are  relatively  few,  whereas  the  points  of  distribu- 
tion of  food  colors  are  very  many,  the  former  being  less  than  20  and 
probably  fewer  than  10,  while  the  latter  may  number  up  into  the 
hundreds;  therefore,  not  only  is  the  labor  and  the  expense  of  quality 
control  of  food  colors  reduced  to  its  probable  minimum  by  keeping 
food  colors  off  the  market  until  they  have  shown  their  right  to  be 
so  used,  but  also  the  certainty  and  the  efficiency  of  quality  control 
is  increased  to  its  probable  maximum. 

The  quality  control  thus  suggested  is  similar  to  that  exercised  by 
the  States  of  New  York,  Michigan,  and  Ohio  over  salt  before  it 
enters  the  market  for  human  consumption.  The  method  of  color 
control  here  suggested  differs  only  in  degree,  not  in  kind,  from  the 
quality  control  exercised  over  salt  by  the  States  named.  Experience 
has  shown  such  quality  control  of  food  colors  to  be  not  only  practi- 
cable but  capable  of  realization  without  any  hardship  and  but  Little, 
if  any,  inconvenience  to  those  concerned. 

STATE  LAWS  PROHIBITING  THE  USE  OF  COLORS  IN  CERTAIN 

FOODS,  1909. 

The  laws  of  the  individual  States  of  the  United  States  have  also 
restricted  the  use  of  coal-tar  coloring  matters  in  foods.  These 
restrictions  are  directed  principally  against  the  use  of  color  to  con- 
ceal inferiority,  which  restriction  is  found  in  almost  all  the  States. 

The  sale  of  poisonous  coloring  matters  for  foods  is  prohibited  in  the 

State  of  New   York,  and  in  New  York  and  North  Carolina  the  addition 

of  injurious  colors  to  foods  is  prohibited. 

Minnesota  and  North  Carolina  prohibit  coal-tar  dyes  in  all  foods. 

Foods  and  beverages  are  considered  adulterated  in  North  Dakota 
and  Wyoming  if  they  contain  aniline  dyes  or  other  coal-tar  dyes. 

Artificial  coloring  is  prohibited  in  sausages  bj  Colorado  and 
Wisconsin. 

Artificial  coloring,  including,  of  course,  coal-tar  color-,  must  not  he 
added  to  vinegar  in  the  States  of  Arkansas,  California.  Connecticut. 

Iowa,  Minnesota,  Missouri,  New  Jersey,  New  fork,  Pennsylvania, 
Tennessee,  Wisconsin,  and  Wyoming. 


42  COAL-TAR   COLORS  USED   IN   FOOD   PRODUCTS. 

Distilled  vinegar  must  not  contain  artificial  color  in  Ohio  and 
Oklahoma,  and  must  be  free  from  harmful  artificial  coloring  matter 
in  Utah. 

In  South  Dakota  oleomargarine  must  not  be  colored. 

Artificial  coloring  is  prohibited  in  milk  by  California,  Oklahoma, 
Pennsylvania,  Utah,  and  Wisconsin  and  in  cream  by  California 
Connecticut,  Pennsylvania,  Utah,  and  Wisconsin. 

Coal-tar  dyes  are  inhibited  in  cakes,  crackers,  candy,  ice  cream, 
and  like  products  by  Virginia.  Ice  cream  is  considered  adulterated 
in  Michigan  if  it  contains  harmful  colors. 

Forty-six  States  prohibit  the  use  of  poisonous  colors  in  candy. 
They  are  as  follows:  Alabama,  Arkansas,  California,  Colorado,  Con- 
necticut, Delaware,  District  of  Columbia,  Florida,  Georgia,  Idaho, 
Illinois,  Indiana,  Iowa,  Kansas,  Kentucky,  Louisiana,  Maine, 
Maryland,  Michigan,  Minnesota,  Missouri,  Montana,  Nebraska, 
Nevada,  New  Hampshire,  New  Jersey,  New  York,  North  Carolina, 
North  Dakota,  Ohio,  Oklahoma,  Oregon,  Pennsylvania,  Philippine 
Islands,  Porto  Rico,  Rhode  Island,  South  Carolina,  South  Dakota, 
Tennessee,  Texas,  Utah,  Vermont,  Virginia,  Washington,  Wisconsin, 
and  Wyoming. 

VI.   RECOMMENDATIONS   BY  ASSOCIATIONS  AND   INDIVIDUALS 
AS  TO  USE  OF  COAL-TAR  DYES  AS  FOOD  COLORS. 

CAZENEUVE  AND  LEPINE. 

Cazeneuve  and  Lepine  (Bull,  de  Vacad.  de  medicine,  April  27,  1886, 
p.  643)  says: 

We  have  arrived  at  the  following  conclusions: 

1.  The  nitro  derivatives  are  especially  poisonous  (dinitronaphthol  being  comparable 
with  picric  acid),  but  the  sulphonated  product  is  harmless. 

2.  Safranin  and  Methylene  Blue  are  harmful,  producing  gastric  intestinal  dis- 
turbances, being  violent  poisons. 

3.  The  following  coloring  matters  are  tolerated  by  man,  whether  well  or  affected 
with  ISright's  disease;  similarly,  too,  animals  (dogs,  guinea  pigs)  without  any  noticeable 
disturbances  and  al  rather  high  doses: 


Probable 

1  trees  Table 

Nos. 


Probable 

Green  Table 

Nos. 


5.  Ponceau  11 55 

6.  Orange  1 85 

7.  Fuchsin  S 462 


1.  Fast  Yellow 9 

2.  Etoccellin 102 

;.  Bordeaux  B 65 

1.    Purple KM)  or  107 

Among  the  nontoxic  Bulphonated  colon  we  have  been  able  t<>  make  out  the  following 
li-t  <-r  classification,  baaed  upon  their  power  of  producing  disturbances,  proceeding 
from  tie-  least  Ineri  to  the  meet  inert: 

Probable 

Qreen  i  able 

Nos. 

...  Yellow  NS 4 

6.  Fast  Yellow 9 

7.  Purph' 106  or  107 


Probable 
i  i  able 
Nos. 

1. 

<  hrange  1 

86 

2 

1  '>'  >rdeaux  l '» . 

68 

A. 

Pom  eau  R 

55 

4. 

•llin 

102 

RECOMMENDATIONS   BY   ASSOCIATIONS,   ETC.  43 

The  results  of  our  experiments  have  led  us  to  the  following  conclusions: 

1 .  The  relative  nonpoisonous  nature  of  the  azo  colors  used  for  coloring  wines  explains 
why  this  artificial  coloring  has  not  caused  any  real  epidemic. 

2.  This  artificial  coloring  of  wines  by  coal-tar  colors  is  dangerous.  It  opens  the  door 
to  the  employment  of  coloring  matters  of  very  variable  and  noxious  properties.  Thus 
Martius  Yellow,  which  is  poisonous,  has  been  used  for  10  years  past  to  color  pastry 
(3  grams  per  100  kilograms)  and  it  may  be  used  to-morrow,  perhaps,  to  color  wines  mixed 
with  a  red  or  a  blue. 

3.  A  rigid  law  against  the  artificial  coloring  of  wines  ought  to  be  promulgated, 
particularly  if  this  coloration  covers  detestable  practices  most  prejudicial  to  the  public- 
health.  The  addition  of  salicylic  acid,  glycerin,  and  tartaric  acid,  or  the  acidifying 
by  sulphuric  acid,  is  cloaked  by  the  use  of  the  coloring  matter. 

Some  sulphonated  azo-coloring  matters  are  sufficiently  inert  to  enable  their  being 
employed  as  artificial  color  in  foods,  bonbons,  and  liquors.  These  colors  are  manu- 
factured according  to  simple  processes  which  give  theoretical  yields  and  no  metallic 
salt,  such  as  mercury,  tin,  or  arsenic  participates;  Btllpha  is  the  only  impurity. 

In  view  of  the  great  extent  of  the  use  oi  these  coloring  matters,  it  is  better  to  regulate 
their  consumption  by  tolerating  certain  of  these  products  rather  than  to  interp' 
illusory  barrier  to  their  use.     'Where  you  can  not  arrest  a  stream  you  can  at  least  regu- 
late its  coui 

It  would  be  better  definitely  to  classify  these  substance.-  with  respect  to  their  noxious 
properties,  tolerate  some  and  prohibit  the  others,  rather  than  to  be  exposed  to  the 
consequences  of  permitting  manufacturers  to  introduce  into  food,  without  any  scien- 
tific control  whatever,  any  products  whatever. 

These  coloring  matters  should  be  sold  in  commerce  under  the  names  of  harmless 
colors  as  determined  by  analysis.  By  chemical  analysis  it  would  be  recognized  as  to 
whether  we  were  dealing  with  one  color  or  with  a  mixture  of  two  or  three  colors. 

The  colors  most  used  are  made  up  of  red,  yellow,  and  blue,  which  apparently  imitate 
the  appearance  of  the  wines  of  the  Midi.  Thus  we  have  recognized  such  coloring 
matters  in  Roccellin,  Xaphthol  Yellow,  and  Methylene  Blue. 

Sulphonated  Fuchsin  is  very  much  used,  combined  with  a  yellow  and  a  blue.  This 
mixture  turns  green  with  ammonia,  like  the  coloring  matter  of  wine.  In  fact,  A.  id 
Fuchsin  is  decolorized  by  ammonia.  The  yellow  and  blue  remain  intact,  and  give  a 
green  which  suggests  true  wine  color. 

SOCIETY  OF  SWISS  ANALYTICAL  CHEMISTS. 

In  1891  the  Society  of  Swiss  Analytical  Chemists  recommended 
that  certain  coloring  matters  which  are  to  be  regarded  as  harmful 
to  health  should  not  be  permitted  to  be  used  in  the  preparation  of 
articles  of  food  intended  for  sale  in  which  artificial  coloring  is  at  all 
permitted. 

The  coal-tar  colors  thus  prohibited  arc  identified  in  the  following 
by  their  Green  Table  numbers,  only  one  trade  name  being  given: 
Picric  Acid  (l);  Dinitrocresol  (2)j  Martius  Yell-.  Aurantia 

Orange    II    (86);  Metanil    Yellow    (95);  Safranin    (584  ;  Methylene 
Blue  (050).     (Zts.  Nahr.  Unters.  Hygiene,  1891,  v. 

TSCHIRCH. 

In  L893  Tschirch  recommended  as  follows: 

1.  Tie-  00tl-tU  OOloiB,  and  in  a  narrow  MOM  the  anilin  ColoiB,  arc  DO  longGf  harmful 

on  account  oi  then*  arsenic  content,  since  at  the  present  time    ■  majority  of 

them  arc  prepared  free  from  arsenic. 

2.  Some  colors  have  shown  themselves  to  be  harmful  to  the  system. 


44  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

3.  Coal-tar  colors  in  general  should  therefore  be  permitted  for  the  coloring  of  foods, 
but  those  that  have  been  found  to  be  harmful  should  be  expressly  and  specifically 
forbidden. 

4.  The  amount  of  coloring  matter  which  has  been  determined  quantitatively  in 
bonbons  and  liqueurs  is  so  small  that  even  the  ones  regarded  as  poisonous  would  not 
be  able  to  develop  their  harmful  effects.  (Zts.  Nahr.  Unters.  Hygiene  Waarenk., 
1893,  v.  7,  p.  338.) 

KAYSER. 

In  1895  Kayser  expressed  liimself  as  follows : 

As  to  the  poisonous  nature  of  organic  coloring,  and  in  respect  to  their  composition, 
H.  Erdmann  (Pharm.  Centralh.,  1892,  v.  33,  p.  357)  concludes  that  in  general  acid 
iffs  can  pass  as  nonpoisonous;  whereas  in  the  case  of  basic  coloring  matters  it 
is  recommended  to  make  a  physiological  examination  before  using  them  for  the  col- 
oring of  things  in  daily  use,  especially  articles  of  food.  ^Tiether  that  portion  of  that 
view  which  deals  with  acid  dyestuffs  will  retain  unexceptionable  and  positive  validity 
appears  doubtful. 

At  the  present  time,  speaking  generally,  interested  manufacturers  take  the  point 
of  view  that  all  the  coloring  matters  which  are  not  forbidden  in  the  food  law  are  to  be 
regarded  as  permitted.  Whether  this  point  of  view  is  free  from  legal  objection  can 
not  be  discussed  here;  that,  however,  it  can  not  be  accepted  from  a  hygienic  point  of 
view  under  any  circumstances  whatever  does  not  require  any  special  proof  for  those 
conversant  with  the  facts.  The  hygienic  requirements  under  all  circumstances 
can  be  summed  up  in  the  following  rule: 

Every  coloring  matter  is  to  be  regarded  in  every  way  as  suspicious,  so  far  as  its 
harmlessness  is  not  proven  by  experience  or  by  correct  physiological  experiments. 

No  one  can  say  in  advance  that  among  the  colors  which  are  to-day  manufactured 
and  used,  which  are  as  yet  not  called  into  question,  there  are  none  which  p 
distinctly  poisonous  properties.     Correct  examination  of  artificial  coloring  matters  in 
this  direction  is,  as  is  well  known,  even  to  the  present  almost  wholly  lacking.     (Forsch- 
ungsberichte  iiber  Lebensmittel,  etc.,  1895,  Vol.  II,  p.  181.) 

WEYL. 

In  1896  Weyl  expressed  himself  as  follows: 

Since  the  number  of  the  organic  coloring  [natters  already  known  is  a  very  large  one, 
and  since  their  number  is  increasing  daily,  and  it  seems  to  be  unlikely  thai  cadi 
individual  of  these  coloring  matters  will  be  examined  as  to  its  poisonous  nature,  there 
an'  only  two  ways  left  in  which  to  solve  the  question  :.-  to  the  use  of  coloring  matters 
in  the  manufacture  of  food  and  articles  of  daily  use. 

One  of  them,  and  at  the  same  time  the  simplest,  would  be  to  prohibit  the  use  of  all 
coloring  matters  for  the  coloring  of  foods,  etc.     This  rigorous  point  of  view  will  hardly 

be  taken  by  legislators,  because  it  would  he  tantamount  to  the  removal  of  many 
marks  of  differentiation  which  have  become  desirable  and  necessary. 

The  second  way  seems  to  he  (he  much  more  practicable,  and  which  Theodor  Weyl 

proposed  some  I  ime  i 

1 1  con  i  i-^  iii  permit  ling  the  use  of  only  a  definite  number  of  coloring  matter.-,  recog- 
nized ;i-  harmless,  for  the  coloring  of  articles  o!  food,  etc.  Which  coloring  matters 
•  I.--  bo  permitted  is  to  he  determined  by  the  authorities  having  jurisdiction. 
'lie-  same  authoritie  are  :>i  o  to  determine  the  maximum  amount  of  each  coloring 
mailer  uhi<  h  c.m  he  used  for  any  purpose.  New  coloring  matters  can  be  used  <>nly 
for  the  above-mentioned  purposes  when  they  have  been  recognized  a-  nonpoisonous 
after  official  test.    All  permitted  coloring  matters  must  he  also  detectable}  even  in 

small  amounts.     (Httndhuch  <l>  r  llijtjiate,  1896,    Vol.  Ill,  p.  $85.) 


RECOMMENDATIONS  BY  ASSOCIATIONS,   ETC.  45 

NATIONAL  CONFECTIONERS'  ASSOCIATION. 

In  1899  the  National  Confectioners'  Association  of  the  United 
wStates  issued  an  official  circular,  which  has  been  previously  discussed,1 
designating  certain  colors  as  harmful,  and  certain  others  as  harmless; 
the  members  of  each  class  are  given  in  the  following  list,  in  which 
only  one  trade  name  is  given,  the  Green  Table  number  appearing  in 
parentheses  at  the  end  of  that  name. 

Harmful  Organic  Colors. 

Red  colors:  Ponceau  3RB  (163);  Crocein  Scarlet  3B  (160);  Cochineal  Red  A  (106); 
Crocein  Scarlet  7B  (169);  Crocein  Scarlet  0  extra  (164);  Safranin  (584). 

Yellow  colors:  Picric  Acid  (1);  Martius  Yellow  (3);  Acme  Yellow  (84);  Victoria 
Yellow  (2);  Orange  II  (86);  Metanil  Yellow  (95);  Sudan  I  (11);  Orange  IV  (88). 

Green  colors:  Xaphthol  Green  B  (398). 

Blue  colors:  Methylene  Blue  BBG  (650). 

Brown  colors:  Bismarck  Brown  (197);  Vesuvin  B  (201);  Fast  Brown  G  (138);  Chrys- 
oidin  (17,  18). 

Harmless  Organic  Colors. 

Red  colors:  Artificial  Alizarin  and  Purpurin  (534);  Eosin  (512);  Erythrosin 
Rose  Bengale  (520);  Phloxin  (521);  Ponceau  2R  (55);  Bordeaux  B  (66);  Ponceau  2G 
(15);  Fuchsin  S  (462);  Archil  Substitute  (28);  Orange  I  (85);  Congo  R.  Azoru- 

bin  S  (103);  Fast  Red  D  (107);  Fast  Red  (105);  Ponceau  4GB  (13);  Fuchsin 

Yellow  and  Orange  colors:  Xaphthol  Yellow  S  (4);  Brilliant  Yellow  (5);  Fast  Yellow 
(8);  Fast  Yellow  R  (9);  Azarin  S  (70);  Orange  (43). 

Green  colors:  Malachite  Green  (427);  Dinitroeoreeorcin  (394). 

Blue  colors:  Indigo  (689);  Gentian  Blue  (457);  Couplers  Blue  (600). 

Violet  colors:  Paris  Violet  (451   :  Wool  Black  (166);  Azoblue  (287);  Mauvein 

Brown  colors:  Chrysamin  R  (269). 

SCHACHERL. 

Schacherl  in  1903  made  the  following  statement : 

If  coal-tar  colors  are  to  be  permitted  for  the  coloring  of  food,  then,  in  my  opinion. 
it  is  not  right  to  limit  the  use  of  such  to  a  few  coloring  matters,  but  groups  of  coloring 
matters  must  be  permitted  which  are  without  suspicion  from  a  sanitary  standpoint, 
and  which  are  characterized  by  definite  reactions.  Other  groups,  on  the  other  hand. 
which  contain  harmful  or  merely  suspicious  colors,  must  be  absolutely  excluded. 
*  *  *  The  selection  would  be  easily  made  if  sufficient  data  were  at  hand  with 
i  to  the  physiological  action.  Unfortunately  this  is  lacking,  a  circumstance 
which  oeed  do!  be  surprising  in  view  of  the  very  large  number  of  synthetic  coloring 
matters,  since  the  Schultx-Julius  tables  enumerate  881  such  colors.  Unfortunately 
the  experiments  of  Th.  Weyl,  which  were  planned  on  a  I  have  not 

completed,  and  apart  from  isolated  mvestigations  we  are  limited  in  passing  judgmenl 
upon  th<'  most  of  these  colors  to  the  proof  that  to  date  nothing  with  respect  to  harmful 
action  has  become  known.  *  *  *  Consequently  it  is  still  possible  that  one  or  the 
other  coloring  matter  which  may  to-day  be  regarded  as  ab  ion,  or  i  newly 

..•red  coloring  matter  may  possesn  poisonous  properties;  the  1-  mould 

under  all  circumstances  have  the  power  to  exclude  for  use  in  foods  all  suspicious 
combinations,  and  all  such  coloring  matters  as  are  not  easily  distinguishable  from  them. 


46 


COAL-TAB  COLOBS  USED  IX  FOOD  PBODUCTS. 


The  final  recommendations  of  Schacherl  amount  to  permitting — 

1.  All  the  Azo  colors,  Nos.  7  to  393  of  the  Green  Tables,  except  No.  86. 

2.  All  the  Triphenylmethane  colors,  Nos.  427  to  492  of  the  Green  Tables,  except 
the  hydroxyl  derivatives,  which  would  be  Green  Tables  Nos.  433, 484,  485, 486.  and  491. 

3.  All  Pyronins,  Nos.  493  to  527  of  the  Green  Tables. 

4.  All  Oxyketones,  Nos.  537  to  570  of  the  Green  Tables. 

5.  All  Indulins,  Nos.  599,  601,  and  603  of  the  Green  Tables. 

6.  Naphthol  Yellow  S,  G.  T.  No.  4. 

7.  Methylene  Blue,  G.  T.  No.  650. 

The  use  of  all  other  coal-tar  colors  would  best  be  forbidden,  partly  from  hygienic 
and  partly  from  practical  considerations  (rendering  control  more  easy),  until  the 
absolute  harmlessness  of  the  group  in  question  is  determined  by  physiological  test. 
*  *  *  It  should  be  required  of  all  permitted  coloring  matters  that  they  shall  not 
contain  substances  which  are  harmful  to  health,  or  even  suspicious,  either  in  chemical 
union  or  as  contaminations.  (Fifth  International  Congress  of  Applied  Chemistry,  Ber- 
lin, 1903,  Vol.  IV,  pp.  1041-1048.) 

The  exclusions  recommended  are  all  nitro-colors,  except  Naphthol 
Yellow  S;  all  acridin  colors  and  all  chinolin  colors;  Auramin,  In- 
dophenol  and  all  nitro-colors,  except  Naphthol  Yellow  S,  Schacherl 
regards  as  not  necessary;  further,  he  has  no  knowledge  of  the  physio- 
logical action  of  any  of  the  azoxy  or  the  thiobenzenyl  colors,  and 
aside  from  Methylene  Blue,  he  has  no  knowledge  of  the  physiological 
action  of  the  oxazins  and  thiazins. 

CLASSIFICATION  OF  RECOMMENDATIONS  IN  THE  LITERATURE. 

The  following  table  shows  the  groups  of  coal-tar  colors  of  the 
Green  Table  classification  and  the  Green  Table  numbers  of  the 
members  of  each  of  the  groups,  together  with  the  favorable  or  unfa- 
vorable recommendations  found  in  the  literature  in  regard  to  each 
and  a  statement  as  to  those  regarding  which  no  recommendations 
are  made: 

Tabulation  of  recommendations  found  in  the  literature. 


Group 
num- 
ber. 

Green 

Table 

number. 

Name  of  color. 

Number  of  Individuals 

reported  on— 

Total  number. 

Un- 
favor- 
ably. 

(i) 

Favor- 
ably. 

(2) 

Con- 
flict- 
Injdy. 

(3) 

Re- 
port cl. 

(4) 

Not  re- 
ported. 

1 

1-6.... 

7  L32  . 

390  U6.. 
417  124.. 
425  126.. 

679  816.. 
617  646  . 
649  667  . 

■ 

Nitro..                         

4 
3 

3 

■> 
10 
8 

0 

is 

7 

6 
83 
13 

0 

2 

M'iip>a/.o 

94 

:* 

l'.H 

4 

16 

11 

0 
0 

l 
l 

1 
II 

2 

1 

8 

7 

Btllbene 

17 

H 

8 

1 

r> 

•> 
2 
(i 
2 
2 
2 

a 

i 
i 

.■ 

0 

0 

.") 
0 
0 
1 
1 

0 

0 
0 
0 
0 

! 

(t 
8 

i 
0 

1 

0 

•_) 
0 
l 
0 

0 
0 

1 

1 
is 
8 
2 
1 
3 
7 
9 
4 
1 
1 

2 
2 

1 

10 

is 

11 

12 

Xanthi                            

27 

1 

13 

1 1 

Anthracene 

88 

us 

81 

80 

17 

B 

5 

1  | 

3 

Sulphlda 

L9 

21. 

5 

Total 

33 

32 

41 

106 

689 

RECOMMENDATIONS   BY   COLOR  INDUSTRIES.  47 

CONCLUSIONS. 

Applying  the  Schacherl  rule,  "Other  groups  which  contain  harmful 
or  merely  suspicious  colors  must  be  absolutely  excluded,"  to  this 
table  and  assuming  that  all  entries  in  columns  1  and  3  shall  be 
regarded  as  rendering  such  colors  as  "harmful  or  merely  suspicious," 
it  will  be  found  that  only  one  group,  namely  the  Stilbene  group, 
would  be  permitted  under  that  rule;  further,  that  tins  rule  would 
admit  17  colors,  not  one  of  which  has  been  reported  on  in  the  litera- 
ture as  to  its  physiological  action.  This  state  of  affairs  tends  to  em- 
phasize the  difficulties  in  the  way  of  any  generalization  which  will  be 
safe  so  far  as  public  health  is  concerned  and  fair  to  those  who  use 
food  colors  for  admittedly  legitimate  purposes  and  to  make  the 
following  recommendation  appears  to  be  the  only  satisfactory  way 
of  solving  the  food-color  problem : 

Although  it  would  be  possible  to  draw  quite  reliable  conclusions  as  to  the  advisa- 
bility of  employing  certain  colors  for  food  products  on  the  basis  of  their  chemical 
constituency,  the  mode  of  their  manufacture  and  of  the  ingredients  used  in  same, 
nevertheless,  I  think  that  by  far  the  safest  way  would  be  on  the  one  side  to  force 
the  dealers  of  colors  intended  for  food  products  to  sell  only  such  colors  with  which 
exhaustive  and  careful  physiological  tests  have  been  made  by  experienced  and  espe- 
cially impartial  and  thoroughly  reliable  people,  thereby  establishing  their  harmless- 
ness  beyond  a  doubt.  On  the  other  hand,  the  manufacturers  and  canners  of  food 
products  of  any  description  should  be  forced  to  purchase  and  use  only  those  colors 
which  they  are  sure  have  been  submitted  to  such  careful  tests  as  have  been  described 
and  by  these  testa  found  to  be  harmless.  (Licbcr,  The  use  of  coal-tar  colors  in  food 
products,  1904,  p.  150.) 

This  view  is  confirmed  by  Santori '  (Moleschott's   Uniersuchungen, 

1895,  Vol.  XV,  p.  57),  who  says: 

From  all  these  experiments  it  follows  that  it  is  impossible,  as  some  have  desired  to 
do,  to  conclude  simply  from  the  chemical  composition  and  constitution  whether  any 
given  coal-tar  dye  is  poisonous  or  nonpoisonous.  Tims  [ndulin  belongs  to  the  same 
group  as  Printing  Blue  and  Methyl  Violet  to  the  same  group  as  does  Acid  Violet; 
therefore  each  individual  coal-tar  dye  must  be  separately  examined,  and  it  is  only 
by  this  laborious  method  that  tie1  use  of  all  really  poisonous  coal-tar  dyes  will  be 
prevented. 

VII.  RECOMMENDATIONS  MADE  BY  UNITED  STATES  COLOR 
INDUSTRIES  AND  TRADES  TO  THE  DEPARTMENT  OF  AGRI- 
CULTURE. 

Prior  to  the  issuance  of  any  regulations,  the  commission  on  rules 
and  regulal  ions  f'<>r  the  food  and  drugs  act .  June  30,  1906,  held  meet- 
ings in  New  York  City  during  September  of  thai  year.  The  steno- 
graphic reports  of  those  meetings,  and  the  briefs  Bled,  in  so  Far  as  ihev 


'Santori  examined  1.'  dilTeretit  Hue  and  violet  dyes  on  dop  by  the  month  and  hypodermic*] 
the  month  and  7  OOUS  by  the  mouth,     lie  found  Indulm  to  ' 

onous  and  Printing  Bhn  to  be  nonpoJeooooj;  ktU  Vlotol  to  be  nonpoiei 

poisonous. 


48  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

relate  to  colored  food,  colored  food  products,  or  material  for  coloring 
foods  or  food  products,  have  been  condensed  verbatim  in  the  following 
pages  with  the  sole  exception  of  omissions,  as  indicated ;  for  obvious 
reasons  the  names  of  those  making  the  suggestions  hereinafter  quoted 
are  not  given.  This  review  of  opinions  expressed  and  recommenda- 
tions given  by  the  industries  and  trades  most  interested  in  the  manu- 
facture, use,  and  sale  of  food  colors  and  colored  food  products  is 
believed  to  be  fair  and  full  with  respect  to  each  and  every  quotation. 
The  numbers  in  parentheses  following  each  quotation  refer  to  the 
pages  in  the  stenographic  minutes  of  the  hearing  from  which  those 
quotations  are  made. 

ANTAGONISTIC  TO  ALL  ADDED  ARTIFICIAL  COLOR. 

1.  Our  position  in  the  coloring  question  is  that  we  are  opposed  to  all  artificial  coloring 
matter  in  food  products.     *    *    *     (p.  109). 

2.  Secondly,  speaking  first  of  our  own  business,  and  I  believe  that  my  view  would 
hold  as  regards  all  food  products,  it  is  my  opinion  that  all  added  artificial  coloring 
matter  in  food  products  should  be  prohibited.  My  experience  in  our  line  of  business 
demonstrates  this  to  me  beyond  any  question  of  doubt  (p.  439). 

CONCERNING  RESTRICTIONS  AND  REQUIREMENTS. 

WHAT    CLASSES    OF   COLORS    SHOULD    BE    PERMITTED   TO    BE    USED. 

1.  All  colors,  irrespective  of  their  class,  whether  animal,  vegetable,  or  synthetic, 
which  have  been  physiologically  and  chemically  examined,  and  which  will  neither 
retard  digestion  nor  have  special  physiological  effects  when  consumed  in  quantities 
corresponding  to  two  grains  per  day  per  adult  (p.  106). 

2.  On  the  use  of  colors  we  recommend  that  any  kind  of  a  harmless  color  should  be 
permitted  provided  it  is  not  a  color  generally  known  to  be  poisonous,  or  generally 
found  to  be  poisonous,  or  one  that  may  be  almost  impossible  to  be  produced  without 
containing  some  poison  within  itself,  when  finished  and  ready  for  use  (p.  119). 

3.  Only  such  colors  as  are  guaranteed  to  be  harmless  by  reliable  manufacturers  should 
be  used  in  the  manufacture  of  confectionery  (p.  555). 

WHY   COAL-TAB    COLORS    SHOULD   NOT   BE    BARRED. 

1.  Coal-tar  colors,  as  a  class,  should  not  be  prohibited;  but  all  those  coal-tar  colors 

generally  found  to  be  poisonous,  or  which  are  hard  to  produce  without  containing 

poisonous  properties  when  ready  ionise,  should  he  forbidden  the  privilege  of  being  used 

or  offered  for  sale  for  use  in  food  (pp.  lit;,  117). 

5.   I  ought  to  put  in  a  plea  for  the  use  of  coal-tar  colors,  harmless,  of  course,  for  the 

i  that  we  have  nol  as  yet  been  able  to  find  any  vegetable  coloring  that  is  suitable 

that  will  give  us  the  results  that  we  require.    Goal-tar  colon,  as  everybody  knows, 

iich  stronger  and  are  more  soluble  and  nol  acted  upon  by  acids,  whereas  the 

table  colors,  with  but  one  exception,  which  is  a  dark  red,  we  have  found  great 

difficulty  in  making  use  of  fox  bottled  soda  water.    Almost  all  the  vegetable  colors 

either  fade  out  or  change  on  accounl  of  the  citric  acid  in  the  syrup  or  food,  or  form  in  a 

little  while  B  precipitation  which  renders  the  foods  unsalable  (pp.  1  L9,  120). 

0.  *  *  *  aniline  butter  colorings  *  *  *  are  superior  to  all  vegetable  colon 
in  the  following  points:  (1)  Shade  and  brilliancy.  (2)  Strength,  by  which  less 
foreign  material  is  introduced  into  the  butter.  (3)  Permanency  when  exposed  to 
Light  and  cold  storage.    I  i)  No  effect  on  the  taste  or  flavor.    (5)  A  clear  solution 


RECOMMENDATIONS   BY   COLOR   INDUSTRIES.  49 

without  sediment  or  mud  which  gives  the  butter  a  uniform  tint  without  specks  (pp. 
176,  177). 

7.  We  recommend  *  *  *  that  the  use  of  harmless  coal-tar  colors,  such  as 
chrysoidine,  tropseoline,  azoflavine,  rocelline,  ponceau,  Bordeaux,  Biebrich  red, 
sulphonated  fuchsin  and  naphthol  yellow  S  be  allowed,  subject  to  declaration  on  the 
label  of  the  quality  and  quantity  of  the  color  used  (p.  226). 

RELATION    OF    LABEL   TO    COLORED    FOOD    PRODUCTS. 


*      ■*       * 


if  it  seems  wise  in  the  opinion  of  the  commission  to  allow  certain  color- 
ing matters  in  food  products,  then  the  names  of  the  coloring  matter  ought  to  be  stated 
on  the  article  (p.  109). 

9.  *  *  *  I  suggest  that  the  use  of  aniline  colors  should  be  made  proper  if  it  is 
so  stated  on  the  label  (p.  127). 

10.  We  recommend  *  *  *  that  the  use  of  harmless  coal-tar  colors  *  *  *  be 
allowed  subject  to  declaration  on  the  label  of  the  quality  and  quantity  of  the  color 
used  (p.  226). 

LABELING    OF   FOOD   COLORS   AS   DISTINGUISHED    FROM    COLORS    FOR   OTHER   USES. 

11.  We  recommend  that  if  by  any  means  the  Government  has  the  power  under 
the  food  laws  to  compel  color  manufacturers  so  to  do,  they  be  compelled  to  label  all 
packages  containing  colors  intended  to  be  used  in  articles  of  food  as  colors  intended 
for  such  purposes  as  distinguished  from  colors  intended  for  other  purposes;  *  *  * 
(pp.  555,  555a). 

THE    TEST   OF    A    HARMLESS    COLOR. 

12.  A  harmless  color  is  one  "which  will  neither  retard  digestion  nor  have  special 
physiological  effects  when  consumed  in  quantities  corresponding  to  two  grains  per 
day  per  adult"  (p.  106). 

QUANTITY    OF   COLOR   TO    BE    CONSIDERED    IN    DETERMINING    HARMLESSNESS. 

13.  The  quantity  of  2  grains  is  mentioned  here  because  in  confectionery  where 
these  harml i   -  colon  are  more  used  perhaps  than  in  any  other  product,  it  would  be 
a  proportion  of  one  part  of  color  to  3,500  parts,  representing  1  pound  of  color  to 
pounds  of  confectionery,  and  that  is  why  that  was  accepted,  because  that  is  practi- 
cally the  maximum  quantity  used  in  confectionery  (p.  106). 

14.  In  the  very  minute  quantities  in  which  the  colors  are  used  in  carbonated  bev- 
-.  it  would  seem  a  great  hardship  to  prevent  us  from  using  coal-tar  colors.    One 

ounce  of  coal-tar  red  will  color  satisfactorily  from  l.dOO  to  2.000  gallon-  of  soda  water. 
<  >i  yellow  and  orange  1  ounce  will  color  from  1,000  to  8,000  gallons.  It  is  readily 
leen  that  unless  the  coloring  used  is  absolutely  a  violent  poison  it  can  have  abso- 
lutely no  effect  on  the  consumer  who  takes  it  in  an  frounce  glass,  and  who  could 
not  possibly  consume  ball  •  gallon  or  a  gallon  of  that  product  (p.  l  L9  . 

15.  On  this  basis  1,000  pounds  of  butter  would  contain  420  grains  of  aniline  color 

lc  <  foe  ounce  of  (dor  to  30  pounds  colored  food  ip.  135). 

■i  hi     MMiilli   in     on  I  I  ki  \  I    COAL-TAB   COD  [BED. 

17.  And  if  I  were  on  this  committee  I  would  advocate  taking  out  two  or  three 

mi-  which  beyond  any  shadow  of  doubt  are  harmless,  and  which  have  been 

experimented  upon,  and  which  would  !»«■  Nuflk-iem  for  all  the  purpose-  nf  the  industry 

*    *    *    none  of  these  colon  are  patented,  anybody  can  manufacture  them  (pp. 

147,  I 

■  i       Bull.  L47— 12 4 


50  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

18.  You  have  been  told  that  the  food  commission  of  the  State  of  Pennsylvania  is 
going  to  rule  that  seven  colors  shall  be  allowed  in  the  State  of  Pennsylvania.  That 
is  not  enough,  because  it  is  not  possible  to  reproduce  all  of  the  required  shades  with 
those  colors  unless  you  take  the  seven  primary  colors,  when  you  can  reproduce  any 
colors.  But  it  is  absolutely  necessary  to  have  about  three  yellows  to  meet  the  require- 
ments of  the  trade.  Some  of  the  articles  that  are  put  out  have  an  organic  acid  nature, 
and  the  anilines  will  stand  that.  *  *  *  On  that  account  the  character  of  the 
food  product  must  be  taken  into  account  in  the  use  of  the  color,  and  the  confectioners 
have  about  30  colors  that  I  know  positively  of    *    *    *    (p.  160). 

19.  We  recommend  that  *  *  *  chrysoidine,  tropaeoline,  azoflavine,  rocelline, 
ponceau,  Bordeaux,  Biebrich  red,  sulphonated  fuchsin,  naphthol  yellow  S  be 
allowed     *    *    *    (p.  226). 

MANUFACTURING   REQUIREMENTS    WHICH   COAL-TAR   COLORS   MUST  FULFIL. 

20.  Coal-tar  colors,  as  everybody  knows,  are  much  stronger  and  are  more  soluble 
and  are  not  acted  on  by  acids.  *  *  *  Almost  all  the  vegetable  colors  either  fade 
out  or  change  on  account  of  the  citric  acid  in  the  syrup  or  food,  or  form  in  a  little 
while  a  precipitation  which  renders  the  goods  unsalable  (p.  119). 

21.  There  are  many  of  these  colors  (coal-tar  colors)  that  will  not  stand  the  natural 
acids  produced  in  manufacturing  foods.  For  instance,  in  making  confectionery,  in 
boiling  candy  you  make  a  certain  grade  of  candy  where  the  mixture  is  boiled  to 
230°.  A  certain  color  will  stand  that  temperature.  Then  you  take  another  candy 
and  that  is  boiled  to  320°  or  340°  F.,  and  the  colors  that  will  stand  230°  will  in  many 
cases  not  stand  the  temperature  of  340°,  while  another  class  of  colors  will  stand  that 
temperature.  So  you  have  got  to  distinguish  and  get  a  color  that  will  stand  these 
difficult  requirements  (pp.  159,  160). 

GUARANTEES   AND   GOVERNMENT  CONTROL. 

22.  Only  such  colors  as  are  guaranteed  to  be  harmless  by  reliable  manufacturers 
should  be  used  in  the  manufacture  of  confectionery  (p.  555). 

23.  We  recommend  *  *  *  that  the  Government  procure  samples  of  such  colors 
from  time  to  time,  wherever  they  have  jurisdiction  so  to  do,  and  if  such  colors  be  not 
legal  for  such  purposes  under  the  food  law,  that  the  6ame  be  prosecuted  and  driven 
off  the  market  in  so  far  as  the  Government  has  the  power  to  do  so;  and  if  no  means 
can  be  devised  to  compel  such  labeling  of  colors  intended  for  food  proposes,  then 
that  the  Government  procure  such  evidence  as  possible  as  to  the  purpose  for  which 
a  color  is  intended  to  be  used,  and  if  such  evidence  shows  a  food  purpose,  that  such 
color  be  prosecuted  if  illegal  under  the  food  law  (pp.  555,  555  a). 

24.  See  page  13. 

25.  The  chemical  test  is  the  first,  and  that,  might  throw  out  a  color  on  account  of 
its  containing  a  little  tin  or  zinc,  or  some  substance  foreign  to  the  food  product. 
Whether  thai  is  deleterious  in  the  quantity  in  which  it  is  present  or  not  is  immaterial 
(p.  160). 

26.  In  a  brief  hied  the  following  suggestions  were  made: 

It  must  be  stated  that  all  the  chemist  can  determine  is  whether  or  nol  the  colors 
contain  some  impurities  that  are  known  to  be  of  poisonous  nature.  Aniline  colors  are 
or  can  be  made  entirely  free  of  such  impurities,  and  with  this  fact  established  the  task 
with  the  chemist  Is  exhausted.    When  it  comes  to  decide  the  question  whether  or  not 

a  color  by  itself,  when  free  Of  all  impurities,  is  injurious  to  health  or  not,  then  the 

chemist  is  not  the  proper  authority;  it  is  for  the  physiologist  and  fox  the  medical  pro- 
tops  i  on  such  questions.  Chemical  theories  go  for  nothing  in  deciding  such 
questions.  It,  would  ool  even  do  to  classify  colors  or  other  substances  according  to 
their  makeup,  ai  it  has  been  shown  again  and  again  thai  substances  belonging  to  the 
same  chemical  class  are  entirely  different,  In  regard  to  the  physiological  conduct. 


INVESTIGATIONS   ON   HAKMFULNESS.  51 

Reliable  information  on  this  subject  can  be  gained  only  by  physiological  experiment, 
as  we  can  not  say  definitely  whether  a  substance,  color  or  any  other,  is  injurious  or 
not  without  finding  out  for  every  substance  by  experiment.  This  has  been  done  for  a 
considerable  number  of  aniline  colors,  and  these  experiments  are  the  only  things  that 
deserve  any  attention.  Everything  else  is  idle  talk.  *  *  *  There  are  a  very 
large  number  of  aniline  colors  that  have  not  been  treated  yet,  and  we  are  safe  in  saying 
that  among  these  will  be  also  some  harmless  and  others  injurious.  As  they  have  not 
been  experimentally  tested,  we  do  not  know  which  are  harmless  and  which  are  not; 
It  will  therefore  be  clear  that  a  law  forbidding  the  indiscriminate  use  of  aniline  color 
for  the  purpose  of  coloring  articles  of  food  is  necessary  and  useful. 

But  if  the  meaning  of  the  law  is  to  prevent  only  the  use  of  injurious  colors,  as  it 
appears  to  be,  then  the  way  to  proceed  would  be  very  definitely  outlined.  Besides 
physiological  colors,  all  such  colors  should  be  forbidden  that  have  been  found  to  be 
injurious  and  such  aniline  colors  as  have  not  been  tested  sufficiently.  There  will 
then  be  left  over  a  number  of  aniline  colors  which  have  been  proven  by  experiment 
to  be  entirely  harmless,  even  if  taken  in  large  doses. 

The  experimenters  were  quite  impartial.  They  had  no  preconceived  ideas,  but 
started  simply  to  find  out  the  true  state  of  affairs.  Their  reports  are  therefore  very 
reliable,  and  it  will  not  do  to  overlook  or  to  ignore  them.  The  colors  that  they  found 
harmless  can  be  considered  perfectly  safe,  so  much  the  more  as  the  doses  conveniently 
taken  with  food  would  be  much  smaller  than  the  doses  that  have  proven  to  be  harm- 
less. These  harmless  aniline  colors  carry  all  the  shades  wanted  in  the  food  industry. 
The  law  should  provide  that  one  of  these  colors  (or  mixtures  of  these)  must  be  used 
when  a  food  article  is  being  colored,  because  these  few  aniline  colors  are  the  only 
colors  that  can  be  considered  perfectly  safe  as  far  as  our  present  knowledge  goes. 
Nothing  should  be  left  to  guesswork  or  experimenting,  as  is  the  case  just  now.  The 
colors  that  are  permitted  should  be  enumerated  by  their  scientific  as  well  as  by  their 
commercial  names,  and  only  such  colors  should  be  listed  as  permissible  for  coloring 
food  products  as  have  been  proven  to  lie  harmless,  even  in  large  doses.  Provision 
should  be  made  to  insure  the  purity  of  the  colors  sold  for  coloring  food;  the  manner 
of  packing  such  colors  and  the  labeling  of  same  should  he  laid  down  clearly,  and  all 
colors  now  listed,  aniline  as  well  as  physiological  colors,  should  be  strict  ly  forbidden. 
If  the  problem  is  viewed  without  preoccupation  and  prejudice,  the  facts  given  above 
will  speak  for  themselves. 

VIII.  INVESTIGATIONS,  OTHER  THAN  ON  ANIMALS,  BEARING  ON 
THE  HARMFULNESS  OF  COAL-TAR  COLORS. 

PFEFFER. 

Pfeffer,  writing    on   the  Absorption   of  Anilin   Colors  by  Living 
Cells,  summarizes  liis  results  as  follows: 

The  relatively  little  poisonous  Methylene  Blue  does  damage  protoplasm  in  a  solution 

of  0.001   percent. 

Methyl  Violet:  This  coloring  matter  i-  not  only  stored  up  in  the  juices  of  the  cell, 

hut  i-  also  able  t<>  color  the  living  protoplasm,  and  care  is  necessary,  on  account  <*"  the 

poic J    nature  <>t"  the  Methyl  Violet,  n>  prevent  damage;  these  caution.-  air  I 

upon  solutions  of  0.0003  bo  0.0000]  |  trength. 

Methyl  Violet  less  poisonous  than  Cyanin. 

Bismarck  Brown  about  as  poisonous  a-  Methylene  Blue. 

ETuchsin  a-  poisonou  ■  as  Methj  lene  Blue. 

Bafranin  a-  poisonoui  as  Methylene  Blue. 

Mnh j  L Oral  |  only  t<>  a  i light 

Tropeeolin  <><  "  in  <><>,  and  Rosolic  Acid  are  not  p 


52  COAL-TAE  COLORS  USED  IN  FOOD  PRODUCTS. 

Methylene  Green  as  poisonous  as  Methyl  Violet. 

Nigrosin  as  poisonous  as  Methyl  Violet. 

Eosin  (Tetraiodo  fluorescein)  kills  in  0.1  per  cent  solution,  but  lets  live  24  hours  in 
0.01  per  cent  solution.  (Untersuchungen  aus  dem  Botanischen  Institut  zu  Tuebingen, 
1886-88,  vol.  2,  pp.  179-331.) 

WINOGRADOW. 

Winogradow  reports  on  the  influence  of  certain  coal-tar  colors  on 
digestion,  which  experiments  were  carried  out  in  glass.  The  con- 
clusions arrived  at  are  as  follows :  ! 

The  twelve  colors,  Safranin  (584^,  Azo  Fuchsin  G.  (93),  Coerulein  S.  (527),  Jodeosin 
(516),  Magdala  Red  (614),  Benzopurpurin  (277,  278,  279,  307),  Ponceau  2R  (55), 
Orange  II  (86),  Phloxin  RBN  (?),  Chrysanilin  (532),  Azoflavin  (92),  and  Cerise 
(mixture  of  448  and  532),  even  in  amounts  of  a  few  milligrams,  which  in  relation  to 
the  digestive  fluid  make  up  only  a  few  tenths  or  hundredths  of  a  per  cent,  exercise  a 
strongly  retarding,  almost  completely  inhibitive,  action  upon  the  peptic  digestion  of 
albumen. 

The  thirteen  colors,  Chinolin  Yellow  (667),  Acid  Green  (434,  435),  Azo  Acid  Yellow 
(92),  Naphthol  Yellow  (4),  Primulin  (659),  Anilin  Orange  (87),  Metanil  Yellow  (95), 
Methylene  Green  (651),  Iodin  Green  (459),  Yellow  T  (84),  Anilin  Green  (?) 
Auramin  O  (425),  and  Martius  Yellow  (3),  retard  the  digestive  action  noticeably, 
although  to  a  slighter  degree  than  the  first  12  colors;  in  any  event  they  are  not  indif- 
ferent.    (Zts.  Ncihr.  Genussm.,  1903,  v.  6,  p.  589.) 

HEIDENHAIN. 

Heidenhain,  in  his  book  entitled  "Ueber  chemische  Umsetzungen 
zwischen  Eiweisskorpern  und  Anilinfarben"  (Bonn,  Germany,  1902), 
reports  on  the  behavior  of  70  different  coal-tar  colors,  3  intermediate 
products,  and  4  raw  materials  toward  various  albuminoids  such  as 
serumalbumen,  albumen,  and  casein. 

Of  these  70  colors,  21  have  been  investigated  physiologically,  and 
the  results  embodied  in  this  report;  and  of  these  21,  17  were  on  the 
United  States  market  as  food  colors  and  4  were  not  on  this  market. 

Limiting  the  attention  to  the  17  that  were  offered,  4  of  them  are 
among  the  7  permitted  colors  of  Food  Inspection  Decision  76. 

In  the  cases  where  albumen  and  casein  were  used,  they  were 
employed  in  0.5,  0.1,  0.02,  0.01,  and  0.005  per  cent  solutions,  acidified 
with  acetic  acid;  the  coloring  matter  was  employed  in  a  1  per  cent 
solution  in  the  Hist  strength,  in  0.1  per  cent  solution  in  tliv  second 
and  third  Strengths,  and  in  a  0.02  pei-  cent  solution  in  the  fourth  and 
fifth  strengths,  and  one  volume  of  coloring-mat  ter  solution  was 
brought  in  contact  with  five  volumes  of  albuminoid  solution. 

The  following  colors  precipitated  the  albuminoid  in  all  the  strengths. 
The  [lumbers   in   parentheses   indicate   the  Green  Table  numbers; 


i  ii  i  po   Ible  to  Identify  the  trade  n  tmei  given  i>y  Winogradow  with  specific  numbers  In 

kbles;  the  anxnben  In  parentheses  after  the  Dame  Indicate  the  number  In  the  Green  Tallies 

wherever  that  identification  oonld  be  made  with  an;  reasonable  certainty;  wherever  two  or  more  numbers 

■  ,  the  context  Indicates  that  the  name  migbl  apply  to  any  one  or  all  of  them. 


INVESTIGATIONS   ON   HABMFULNESS.  53 

the  numbers  in  italics  are  those  of  the  permitted  list  of  Food  Inspec- 
tion Decision  76:  (55)  Ponceau  2  R,  (65)  Fast  Red  B,  (434)  Light 
Green  SF  bluish,  (56)  Ponceau  3  R,  and  (106)  New  Ooccin. 

The  following  precipitated  in  all  but  the  fifth  strength:  (107) 
Amaranth. 

The  following  precipitated  onry  the  first  three  strengths:  (14) 
Orange  G  and  (85)  Orange  I. 

The  following  precipitated  only  the  first  two  strengths:  (462)  Acid 
Magenta. 

For  the  basic  colors  the  method  of  testing  was  different  from  that 
described  for  the  acid  colors  and  the  amounts  employed  were  not  so 
definitely  set  forth.  A  1  per  cent  solution  of  serum  albuminoid  was 
employed;  the  solution  of  coloring  matter  used  varied  in  strength 
from  0.5  to  1  per  cent  (b),  a  "very  dilute  solution"  (a)  being  also 
employed.  The  annotations  given  by  the  author  (p.  114)  are  herewith 
reproduced  in  full : 

(17)  Chrysoidin  Y.     (a)  In  a  very  dilute  solution  the  yellow  base  is  at  once  Liber- 
ated, and  when  sufficient  color  is  added  albumen  precipitation  takes  place.     No  color 
change  on  heating,     (b)  Turns  yellow  at  once.     Further  additional  color  prodi 
brown  and  albumen  precipitation. 

(201)  Manchester  Brown,     (a)  Becomes  yellow  at  once,  due  to  separation  of  the 
free  base.     On  heating  no  change,     (b)  Becomes  a  discolored  brown,  and  prod 
nice  brown  albumen  precipitate. 

(425)  Auramin  0.     (a)  No  change,     (b)  Precipitates  albumen  strongly. 

(427)  Malachite  Green.  (The  oxalate  of  the  color  was  used.)  (a)  Color  changes 
from  a  blue-green  to  a  more  pure  green,  (b)  Cold,  no  precipitation  of  albumen; 
heated,  sudden  precipitation  of  albumen. 

(428)  Brilliant  Green.  (A  sulphate  of  the  color  was  used  Becomes  milky. 
(6)  Immediate  precipitation  of  albumen. 

(448)  Magenta.    (Acetate  and  nitrate  were  used,  and  in  both  acted  the  -aim- 
Color  changes  from  yellowish-red  to  rose-red.     (6)  Albumen  precipitation  abundant, 
ev<n  in  the  cold. 

(451)  Crystal  Violet,  (a)  The  color  loses  its  reddish  cast  and  changes  to  pure  blue. 
(b)  Albumen  precipitated  by  the  use  of  much  color. 

(4)  Naphthol  Yellow  S  was  tested  as  the  free-color  acid  and  not  as  the  sodium  or] 
edum  salt,  which  is  its  commercial  form.     It  precipitated  the  albuminoid  from  the 
following  solutions:  l.  1  per  cent  serum  albumen  in  water.    2.  0.5  per  cent  serum 
albumen  in  io  percent  acetic  acid.    3.  Casein,  0.5  percent  in  1<>  percent  a 

rum  albumen;  5,  I  asein;  <i.  Nfuclein,  all  in  0  ition  In  0.2  per  cent 

sodium  hydroxid.    7.  Nucleinic  acid  in  0.5  per  i  ent  wat<  r  solution, 

The  relationship  between  the  amounts  of  color-acid  and  albuminoid 
Bolution  here  used  docs  not  appear  definitely  in  the  book. 

Baying  reference  now  t<>  the  literature  and  the  physiological 
action,  as  compiled  herein,  it  will  be  observed  that  the  ability  to  pre- 
cipitate albumen,  or  not  to  precipitate  it,  under  the  conditions  <>!' 
Heidenhain,  appears  not  to  have  anj  direct  connection  with  the 
results  obtained  by  actual  physiological  test  <»n  animala  or  num. 
For  instance,  among  the  five  thai  precipitated  all  five  Btrengths  of 


54  COAL-TAB  COLOBS  USED  IN  FOOD  PBODUCTS. 

albumen  and  casein,  No.  65,  Fast  Red  B,  of  the  Green  Tables,  has 
been  found  to  be  not  harmful  by  tests  actually  described;  No.  56, 
Ponceau  3  R,  belongs  to  a  class  of  colors  genericalry  permitted  by  the 
law  of  Austria;  Nos.  55,  Ponceau  2  R,  and  106,  New  Coccine,  have 
been  reported  on  both  favorably  and  unfavorably  by  different  experi- 
menters; No.  434,  Light  Green  SF  bluish  on  physiological  examina- 
tion has  been  described  as  suspicious. 

From  this  it  appears  that  two  colors,  physiologically  probably 
harmless,  precipitated  all  the  five  strengths  of  albumen,  and  three 
colors,  which  are  perhaps  no  more  than  suspicious,  likewise  precipi- 
tated all  five  strengths  of  albumen. 

No.  107,  Amaranth,  which  has  been  examined  with  favorable 
results  by  two  different  experimenters,  precipitates  four  out  of  the 
five  strengths. 

Of  the  two  colors  precipitating  the  first  three  strengths,  both  hare 
been  examined  physiologically  with  favorable  results,  namely,  Nos. 
14,  Orange  G,  and  85,  Orange  I. 

The  color  which  precipitated  only  the  first  two  strengths,  namely, 
No.  4G2,  Acid  Magenta,  has  likewise  been  examined  physiologically, 
and  the  reports  are  favorable. 

Thus  it  would  seem  that  there  is  no  definite  connection  between  the 
physiological  action  and  the  ability  to  precipitate  albumen  from 
acetic  acid  solution  in  the  case  of  acid  colors. 

In  the  case  of  basic  colors  the  situation  seems  to  be  somewhat 
different. 

OTHER  AUTHORS. 

Rosenstiehl  {Fifth  International  Congress  of  Applied  Chemistry, 
Vol.  Ill,  j).  700)  states  that  when  the  color  is  present  in  an  excess, 
yeast  absorbs  8  per  cent  of  Magenta  (448)  and  5  per  cent  of  Malachite 
Green  (427,  428).  The  Acridins  (528-538),  the  Thionins  (649-657), 
the  Safranins  (583,  584),  and  the  Rosanilins  (447-448)  dye  yeast  the 
best;  solutions  containing  3  per  cent  by  weight  of  the  dry  weight  of 
the  yeast  arc  completely  decolorized  by  such  yeast  and  at  ordinary 
temperatures.  The  Eosins  and  Phthaleins  dye  the  yeast  only  incom- 
pletely, whereas  Azo  dyes  (7   393)  (with  the  exception  of  BenzO  PuT- 

purin,  277, 278,  279,  309)  do  not  dye  yeast  at  all.  Such  dyed  yeast, 
however,  is  not,  dead;  it  has  merely  lost  its  power  to  cause  fermenta- 
tion. The  numbers  in  parentheses  are  the  corresponding  numbers  in 
the  Green  Tables  as  nearly  as  they  could  he  identified. 

Bokorny  (CTiem.  ZUj.,  190(J,v.30,i).217)  examined  Magenta  (448), 
Safranin  (584),  Victoria  Blue  (487,  488  or  490),  Methylene  Blue  (660), 
and  Alizarin  Blue  (562  or  563)  (the  numbers  In  parentheses  are  the 
probable  Green  Table  numbers)  as  to  their  effect  on  micro-organisms 
such  as  yeast  Cells,  infusoria,  and  the  like,  and  found  that  these  dyes 


INVESTIGATIONS   ON    HARMFULNESS.  55 

in  a  concentration  of  1:100,000  killed  them,  whereas  strychnin 
nitrate  in  the  same  concentration  is  substantially  without  effect. 
Death  is  caused  by  absorption  of  the  dye  by  the  albumen  of  the 
protoplasm.  The  dyes  seem  to  be  absorbed  not  only  by  living  albu- 
men, but  also  by  living  nerve  cells  and  fibers.  Pure  anilin  or  coal- 
tar  colors,  however,  are  not  poisonous  in  the  ordinary  meaning  of  the 
words,  that  is,  humans  are  not  likely  to  be  easily  injured  by  them. 

Houghton  (/.  Amer.  Cliem.  Soc,  1907,  v.  29,  pp.  1351-1357)  shows 
that  Bismarck  Brown  (197,  201)  and  Crocein  Scarlet  (160?)  hinder 
the  peptic  digestion  of  fibrin,  casein,  and  albumen. 

Stilling  (Anilinfarbstoffe  als  Antiseptica,  1890,  v.  2,  pp.  55-56)  states 
that  he  found  the  animal  cells  to  be  affected  by  pure  coal-tar  colors 
in  the  same  way  that  vegetable  colls  were  affected. 

Penzoldt,  based  upon  the  experimental  work  of  Beckh   {Archiv. 

Exp.  Path.  Pharmak.  1890,  v.  26,  p.  310),  reports  as  follows: 

Of  the  15  dyes — 

Green  Table 
Name.  number. 

1.  Malachite  Green 427 

2.  Hofman's  Violet  (methyl  variety) 450 

3.  Methyl  Violet . 451 

4.  Rose  Bengal  (Erythrosin) 517 

5.  Phenyl  Blue 480 

G.  Methylene  Blue 050 

7.  Fuchsin 448 

8.  Coralline 484 

9.  Eosin 512 

10.  Methyl  Orange 8' 

11.  Vesuvin L97 

12.  Tropaeolin 88 

13.  Scarlet  Red (?) 

14.  Congo  Red 240 

15.  Indulin  eulpho  acid 001 

all  of  which  are  water  soluble  and  when  used  were  free  from  arsenic,  only  the  li 

in  saturated  solution  arrested  the  development  of  Gtaphylococut  pyog<  r,  and 

of  these  six  all  but  the  Erythroaii]  and  Methylene  Blue  arrested  the  growth  of  anthrax 
bacillus. 

Of  these  six  when  injected  into  rabbits  subcutaneously  the  following  produced  no 
changes  of  consequence:  Erythrosin  (250),  Phenyl  Blue  (100  .  Methylene  Blue 
The  numbers  in  parentheses  show  the  number  of  milligrams  of  dye  per  kilo  body 
weight  of  the  rabbit  -. 

Methyl  Violet  (50)  produced  only  local  changes,  sui  h  as  gangrene. 

Malachite  I  Ireen  LOO)  and  Bofman's  Violet  1 20 :  produced  muscular  pararj  sis,  which 
in  the  case  of  Malachite  Green  resulted  fatally  on  the  ninth  day;  in  the  case  of  Sof- 
man'a  Violet  the  paralysis  iras  complete  on  the  tenth  day. 

The  remaining  nine  colors  are  apparently  «>f  do  effect  upon  staphylococui  or  upon 

anthrax 

II.  \Y.  Williams  {A   Manual  of  Bacteriology \  U \  p.  M0),  under 

" Disinfectants  and  Germicides,"  says: 

Aniline  dyes.  Many  of  these  substances,  notably  pyoktanin  (Methyl  Violet  .  pos- 
■ev  germicidal  properties.    A.  solution  of  1:6000  will  sill  the  anthrax  bacillus  in  two 


56  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

hours.  A  much  stronger  solution,  1:150,  is  required  to  kill  the  typhoid  bacillus  in 
the  same  time.  Malachite  Green  is  said  to  possess  even  greater  germicidal  power  than 
pyoktanin.     Methylene  Blue  also  possesses  considerable  germicidal  power. 

IX.  COMPILATION  UNDER  THE  GREEN  TABLE  NUMBERS  OF  ALL 
INFORMATION  AVAILABLE  AS  TO  THE  SUITABILITY  OF  COAL- 
TAR  COLORS  FOR  FOOD. 

GENERAL  STATEMENTS. 

Before  entering  upon  a  detailed  study  of  what  has  been  published 
for  and  against  specific  coal-tar  colors,  it  is  probably  well  to  consider, 
for  whatever  they  may  be  worth,  some  of  the  general  statements  that 
have  been  made,  from  time  to  time,  in  the  literature  relative  to  coal- 
tar  colors,  considered  either  as  a  whole  or  as  subdivisions  or  classes 
thereof,  and  their  physiological  action  or  their  suitability  for  use  in 
foods. 

1.  Schultz  (Die  Chemie  des  SteinkoMenthcers,  Brunswick,  1887-1890, 
Vol.  II,  p.  85),  after  discussing  the  regulations  of  the  German  Empire 
in  respect  to  food  coloring,  says: 

With  respect  to  these  regulations  the  artificial  organic  coloring  matters  can  be 
regarded,  in  general,  as  harmless.  For  the  purposes  of  dyeing  magenta  made  by 
means  of  arsenic  acid,  further  picric  acid,  and  those  coloring  matters  which  occur  as 
oxalates  or  zinc  chlorid  double  salts,  such  as  Methylene  Blue  and  Bitter  Almond  Oil 
Green,  can  be  used.  The  use  of  the  substances  named  for  the  coloring  of  food  products 
is,  however,  suspicious  and  should  not  be  permitted. 

2.  Stilling  (Anilinfarbstoffe  ah  Antiseptica,  Strassburg,  1890,  Vol. 
II,  pp.  55-56)  says: 

In  view  of  the  fact  that  the  most  innocent  substance,  such  as  distilled  water  or  com- 
mon salt,  when  introduced  in  large  quantities  into  the  organism  can  act  fatally,  the 
anilin  coloring  matters  therefore,  particularly  if  they  be  free  from  all  admixtures,  such 
as  arsenic,  copper,  and  chlorid  of  zinc,  are  to  be  regarded  as  wholly  nonpoisonous. 

All  experience  gathered  since  my  first  publication  has  likewise  fully  confirmed  this 
nonpoisonous  nature. 

3.  Stilling  (Ber.  Klin.   Wochensch.  1890,  p.  531)  also  says: 

Proceeding  from  purely  theoretical  views,  and  based  upon  these  botanical  and 
physiological  experiments,  1  have  recommended  anilin  colors  as  antiseptics  for  the 
following  reason-: 

J.  They  are  to  be  designated  as  absolutely  nonpoisonous.  This  will  be  confirmed 
by  every  chemist  acquainted  with  the  relevant  details,  and  also  from  the  medical  side 
this  has  long  ago  been  determined  by  Grandhomme.  The  publications  of  tins  author, 
who  made  extern  i  ire  observations  and  experiments  in  the  anilin  factory  ot'  Heister, 
Lucius  &  Bruening,  appeared  in  the  beginning  of  the  ei|  hi  ies,  and  has  hardly  become 
known  in  medical  circles.  However,  I  was  first  made  acquainted  with  this  by  my 
colleague,  Prof.  Rose,  in  Btrasburg. 

2.  That  ii  Is  possible  to  bring  about  death  in  experimental  animals  by  introducing 
large  amount!  of  the  coloring  matter  into  the  peritoneal  i  a\  ii  >•  proves  nothing  against 


COMPILED  DATA   UNDER  GREEN   TABLE   NUMBERS.  57 

the  nonpoisonous  nature  of  these  substances.  This  action  is  to  be  regarded  as  a  purely 
mechanical  one,  a  view  which  I  will  thoroughly  confirm  in  my  second  communication. 
With  respect  to  the  anilin  colors  not  soluble  in  water,  Ehrlich  long  before  me,  in  his 
excellent  publication  on  the  oxygen  requirements  of  the  organism,  has  arrived  at  this 
view,  and  has  excellently  described  it  as  merely  a  penetration  of  the  organs. 

4.  Lelimann  (Meihoden  der  Praktischen  Hygiene,   Wiesbaden,  1890, 
p.  54-3)  says: 

The  hygienic  significance  of  coal-tar  colors  has  heretofore  been  judged  quite  vari- 
ously. When  the  intensely  poisonous  nature  of  the  first  impure  and  particularly 
arsenic-containing  coloring  matters  became  known  the  inclination  was  to  judge  the 
coal-tar  coloring  matters  very  strictly;  when  it  was  subsequently  recognized  that 
the  contaminations  were  largely  the  cau.se  of  the  harmfulness  to  health,  there  followed 
a  period  in  which  no  poisonous  coal-tar  coloring  matter  was  known  in  any  pure  con- 
dition. (Eulenberg  &  Vohl,  1870.)  More  recent  investigations,  however,  have 
disclosed  a  series  of  coal-tar  coloring  matters  which,  as  a  matter  of  fact,  possess  a  con- 
siderable poisonous  action,  and  already  cases,  although  not  numerous,  have  become 
known  in  which  serious  and  even  fatal  poisonings  by  means  of  pure  coal-tar  colors 
have  arisen.  Alongside  of  this  there  still  continue  to  exist  the  possibilities  described 
by  Eulenberg  and  Vohl  (Viertel-Jahressch.  fur  Gerichtliche  Mediz,  1870),  whereby 
harmless  coloring  matters  become  harmful;  but  the  realization  of  these  possi- 
bilities has  become  essentially  more  seldom  through  improvements  and  chanj 
manufacture. 

5.  Stilling  (Arch.  Exper.  Pathol.  Pharmal.,  1891,  v.  28,  p.  352),  in 
speaking  of  the  anilin  colors  as  antiseptics,  says: 

It  is  the  nonpoisonous  nature  of  these  substances,  their  easy  solubility  and  dif- 
fusibility,  and  above  all  their  inability  to  coagulate  albumen  which  lends  them  their 
importance,  which  now  can  be  only  difficultly  denied. 

Note. — The  work  of  Heidenhain  abstracted  in  Section  VIII  does 
not  fully  bear  out  this  article. 

6.  Erdmann  (Pharm.  d  nfml/i.,  IS!' J,  t>.  38,  p.  ps: 

The  sulphonated  as  well  as  the  carboxylated  coal-tar  dyes  will  not  have  any  pro- 
nounced action  on  the  organism.    Acid  dyea  may  therefore  be  regarded  in  : 
as  nonpoisonous,  whereas  in  the  case  of  basic  dyes  a  physiological  examination  is  to  be 
recommended  before  they  are  permitted  to  be  applied  to  articles  in  daily  use  or 
indeed  to  be  used  in  food  or  drink. 

Note.— Out  of  the  80  different  dyes  on  the  food-color  market  in 
the  summer  of  1907  whose  composition  was  avowed,  i;>  were  basic 

and  65  were  acid. 

7.  Tschirch  expressed  himself  as  follows: 

1.  T  and  in  a  narrower  sense  the  anilin  colon,  arc  no  I 
harmful  on  ao  ounl  of  their  arsenic  content,  since  at  the  j  ties*  ml  time  the  great  majority 
of  them  are              ;.  free  from  arsenic. 

2.  Some  colors  ha\  e  shown  themselves  to  be  harmful  to  the  system 

1  oal-tar  col  aeral,  should  therefore  be  permitted  for  the  coloring  of 

but  those  that  have  been  found  to  be  harmful  should  be  expressly  and  specifically 
forbidden. 


58         COAL-TAB  COLORS  USED  IN  FOOD  PRODUCTS. 

4.  The  amount  of  coloring  matter  which  has  been  determined  quantitatively  in 
bonbons  and  liqueurs  is  so  small  that  even  the  ones  regarded  as  poisonous  would  not 
be  able  to  develop  their  harmful  effects.  {Zts.  Nahrs.  Unters.  Hygiene  Waarenk., 
1893,  v.  7,  p.  338.) 

8.  Georgievics  (Lehrbuch  der  Farbenchemie ,  Leipzig,  1895  p.  10) 
says  under  "Poisonous  nature  of  the  coloring  matters:" 

It  is  a  little  known  fact  that  of  the  very  large  number  of  organic  coloring  matters 
only  a  few  have  been  found  to  be  poisonous;  these  are  Picric  Acid,  Victoria  Orange 
(Saffron-surrogate),  Aurantia,  Metanil  Yellow,  Orange  II,  and  Safranin.  The  preju- 
dice which  is  still  quite  widely  accepted  that  most  of  the  artificial  coloring  matters 
are  poisonous  dates  from  the  early  periods  of  anilin-color  manufacture,  at  which  time 
magenta  and  the  coloring  matters  made  from  it  occurred  in  commerce  highly  con- 
taminated with  arsenic.  At  present,  however,  these  coloring  matters  are  prepared 
absolutely  free  from  arsenic,  and  are,  as  such,  nonpoisonous.  A  few  coloring  mat- 
ters which  occur  commercially  as  zinc  chlorid  double  salts,  such  as  Methylene  Blue 
and  Malachite  Green,  may  be  harmful  in  consequence  of  their  zinc  content,  and 
should  therefore  never  be  employed  in  the  coloring  of  food  products.  *  *  *  In 
consequence  of  their  physiological  activity  some  coloring  matters  are  employed  as 
medicines,  indeed  principally  Methyl  Violet,  Auramin  and  Methylene  Blue.  The 
first  two,  known  as  blue  and  yellow  Pyoctanin  (pus-destroying)  are,  owing  to  their 
great  antiseptic  action  and  diffusibility,  valuable  medicines;  on  account  of  the 
unpleasant  coloring  effect  accompanying  them  they  are  but  little  used.  Methyl 
Violet  was  first  recommended  as  an  antibacterial  remedy  in  diseases  of  the  eye  by 
Stilling;  subsequently  it  has  been  employed  in  other  special  cases;  its  principal 
use,  however,  is  in  surgery  for  the  prevention  of  malignant  proud  flesh. 

The  use  of  Auramin  is  entirely  analogous. 

Methylene  Blue  (as  a  free  base)  is  used  principally  as  an  analgesic  (pain-relieving 
remedy)  and  is  given  internally;  on  account  of  its  ability  rapidly  to  diffuse  through 
the  tissues  of  the  nervous  system;  it  can  also  be  introduced  by  injection.  It  is  used 
as  a  remedy  against  malaria,  carcinoma,  Bright's  disease,  etc. 

The  following  have  been  tested  as  remedies  or  as  antiseptics:  Safranin,  Lydin 
(Mauvein),  Vesuvin,  Anilin  Blue,  Carbolic  Magenta,  Alizarin  Yellow  C  (Gallaceto- 
phenone) ,  etc.  The  potassium  salt  of  Dinitro-ortho-cresol  was  brought  into  com- 
merce by  the  Farbenfabriken  vorm.  Friedr.  Bayer  &  Co.,  under  the  name  of  Anti- 
nonnin,  and  has  given  excellent  results  as  a  means  against  formation  of  mold  in 
cellars  and  against  wood  fungi. 

9.  Weyl  (Handbuch  der  Hygiene,  1896,  p.  378)  says: 

A  few  organic  coloring  matters,  but  only  a  very  few,  possess  poisonous  properties. 
A  rule  by  means  of  which  the  poisonous  or  nonpoisonous  nature  of  organic  coloring 
materials  can  be  determined  without  experiment  is  unknown  even  for  those  coloring 
matters  whose  constitution  has  been  determined  and  experiments  on  the  poisonous 
nut  arc  of  organic  coloring  mat  tor-  an-  very  few  in  number. 

10.  Lewin  {Lehrbuch  der  Toxicologie,  1897,  p.  230)  says: 

In  the  use  ol  various  fabrics  or  of  foodstuffs,  which  are  colored  with  anilin  or 
coal-tar  colors,  or  in  commercial  contact  with  such  colors,  local  and  general  symptoms 

..!'  poisoning,  SUCh   BJ  eczema,  swelling  of   the   face,   vomiting,  diarrhea,  amesthesia, 

paresis,  etc.,  have  been  observed.    The  e  are  generally  duo  to  the  toxic  nature  of 
the  coloring  matters,  frequently  to  harmful  ingredients  of  the  same,  and  hardly  ever 

to  poisonous  mordants.      Many   workmen    in   anilin    factories  -how  permanent    spots; 
nmple,  On   the  cornea  ami  conjunctiva,  head,  Chest)   lace,  ami   neck,  without 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS.  59 

any  interference  with  their  general  condition.  Local  changes  of  more  serious  nature 
have  more  frequently  been  observed  in  the  mucous  membranes  and  on  the  skin. 
Thus,  in  one  case,  a  camel's-hair  pencil,  soaked  with  anilin  color,  accidently  entered 
the  eye,  and  at  first  nothing  was  noticed  but  a  violet  blue  coloration,  later  inflamma- 
ion  and  chemosis  took  place.  I  have  observed  local  swelling  and  indurations  of  the 
skin,  particularly  on  the  cheeks,  in  the  case  of  children  after  they  had  worn  caps 
colored  with  anilin  dye. 

11.  Winton  (Connecticut  Agric.  Eiper.  Sta.  Report,  1901,  p.  181) 
says : 

Although  there  is  evidence  that  most  of  the  coal-tar  dyes  are  not  injurious  to  some 
of  the  lower  animals,  it  is  not  safe  to  assume  that  they  are  entirely  harmless  to  human 
beings.  The  dog,  an  animal  used  in  most  of  Weyl's  experiments,  has  a  proverbially 
strong  stomach,  and  eats  with  no  apparent  discomfort  many  things  which  would 
disturb  the  digestion  of  a  man. 

12.  Chlopin,  in  his  book  published  in  1903  (see  p.  75),  state-  i  - 
follows : 

{Page  114.)    *    *    *    All  the  dyes  examined  by  me  I  divided  into  three  categories: 

Dyes  which  caused  striking  general  symptoms  of  poisoning  and  led  to  the  death  of 
the  animal,  or  would  have  led  to  it  if  the  experiments  were  not  purposely  discon- 
tinued, I  designate  by  the  term  poisonous;  dyes  which  induced  some  separate  and 
temporary  symptoms  of  disease,  for  instance,  vomiting,  diarrhea,  separation  of  albu- 
men in  the  urine,  the  general  condition  remaining  normal,  I  designate  as  suspicious: 
lastly,  the  dyes  which  caused  no  apparent  disturbance  during  the  experiments  are 
designated  by  the  term  nonpoisonous.  I  purposely  do  not  call  the  last  category 
harmless,  because  by  our  experiments  the  question  could  not  be  decided  negatively 
as  to  whether  the  nonpoisonous  dyes  did  not  cause  some  finer  pathological  changes  in 
the  organism  and  functions  which  could  not  be  detected  by  simple  observation. 

(Pages  219-221.)     Thus,  according  to  all  the  investigators  quoted,  there  were  found 
altogether  22  poisonous  and  harmful  dyes,  out  of  about  60  dyes  examined;  which 
makes  30.7  per  cent  of  poisonous  and  harmful  dyes  among  those  examined. 
My  investigations  gave  30  per  cent  of  poisonous  and  40  per  cent  oi  suspicious 
The  percentages  above  given  have  a  fairly  well  established  basis,  since  they  were 
obtained  by  the  examination  of  100  dyes,  which  is  about  one-fifth  ol  all  the  dj 
commerce.     Further,  considering  the  distribution  ol  the  poisonous  and  harmful  dyes 
according  to  various  chemical  groups,  we  find  that  they  occur  in  12  oi  the  L8  groups, 
and  we  can  not  note  any  regularity  in  this  distribution;  ii  is  impossible  to  say  that 
there  is  any  definite  connection  between  the  feci  that  the  dye  belongs  to  a  certain 
chemical  group  and  its  action  on  the  animal  organism.     Usually  among  the  .'. 
one  ami  the  same  group  there  are  some  harmful  one-,  but  there  are  also  some  harmless 
ones,  and  the  ones  and  the  others  have  very  similar  composition.     This  or  that  action 
of  the  dyes  on  the  animal  organism,  as  we  shall  presently  see,  u  d<  termined  m< 

the  delicate  < Inference   in   the   internal   structure  of   their  molecules   than    by   those 

differences  <>n  which  i-  based,  at  the  pi of  time,  the  classification  of  the  aromatic 

dyes. 

On  the  I' .i-i~  of  tin-  whole  experimental  material  on  hand      mine  and  that  of  other 

invest  igatora     I  can  make  only  the  following  very  few  and  purely  empirical  generalisa- 

l .  According  to  the  shade  produced,  the  poisonoui  and  harmful  colors  are  distributed 

ai  follows:  Blosl  "\  all  poisonous  dyes  are  found  among  the  Yellows  and  the  < » ranges; 

then  come  the  Blues,  then  the  I'-'",    -ami  the  BUm  k  ry  few  harmful 

among  the  Violets  and  Qi  found  ool]  picious 

one,  and  DO  poisODOUi  ones. 


60  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

2.  The  most  poisonous  dyes  belong  to  the  Nitro,  Azo,  Tri phenyl,  and  Thiazin 
groups,  and  also  to  the  Auramins. 

3.  A  whole  group  of  poisonous  and  harmful  dyes  is  formed  by  the  new  sulphid  dyes 
known  as  Yidal's  dyes. 

(Page  224-)  By  the  facts  and  observations  quoted  above  is  corroborated  the  opinion 
that  in  general  the  coal-tar  dyes,  according  to  the  composition  and  properties,  appear 
as  substances  foreign  to  the  animal  organism,  and  may  influence  harmfully  the  vital 
functions,  even  in  those  cases  when  they  do  not  possess  distinctly  poisonous  properties. 
For  this  reason  many  hygienists  make  it  a  principle  not  to  allow  the  coloring  of  food 
products  or  of  beverages  with  coal-tar  dyes,  independently  of  the  fact  whether  they 
prove  in  actual  experiments  on  animals  poisonous  or  not. 

We  must  therefore  agree  with  M.  Rudner  that  food  of  the  masses  require  the  most 
far-reaching  protection,  maintaining  them  free  from  foreign  additions. 

13.  Koenig  {Die  Menschlichen  NaJirungs-  und  Genussmittel,  Berlin, 
1904,  Vol  II,  p.  162)  says: 

Even  though  the  majority  of  the  anilin  coloring  matters,  in  view  of  the  small 
amounts  in  which  they  are  generally  employed,  can  not  be  regarded  as  directly  harm- 
ful to  health,  yet  the  objections  to  their  use  in  the  coloring  of  food  products  for  the 
purpose  of  substituting  or  strengthening  a  natural  color  lies  in  the  deception  con- 
nected therewith    *    *    *. 

14.  Fraenkel  (Arzneimittel-Synihese ,  Berlin,  1906,  j).  570)  says: 

It  is  clear  that  the  coloring  property  of  these  chemical  substances  stands  in  no 
relation  to  their  physiological  actions,  but,  on  the  contrary,  the  physiological  actions 
depend  only  upon  the  general  structure  of  these  substances,  and  therefore  upon  their 
membership  in  definite  chemical  groups. 

(Pages  574-5.)  We  see,  even  in  considering  this  group  of  substances,  that  they  do 
not  possess  any  specific  action,  but  they  are  capable  of  use,  preferably  by  external 
application,  as  antiseptic  materials,  as  materials  which  in  their  action  Btand  somewhere 
between  carbolic  acid  and  corrosive  sublimate,  and  whose  coloring  property,  in  conse- 
quence of  which  they  were  primarily  selected,  is  directly  a  hindrance  in  this  use, 
since  the  coloring  of  the  bandages  and  the  hands  of  the  operators  and  the  skin  of  the 
patients  certainly  can  not  be  regarded  as  a  pleasant  occurrence;  that  the  antra  ptic 
action  stands  in  some  relationship  to  the  properties  of  the  substances  as  coloring  matter 
must  be  positively  contradicted.  It  depends  <>nly  on  the  general  structure  of  the 
substance,  and  does  not  stand  in  any  direct  relation  to  the  ehromophore  and  anxo- 
chrome  groups  of  the  substances,  but  more  closely  to  the  aromatic  nucleus.  Indeed, 
it  may  happen  that  an  auxochrome  group  diminishes  the  antiseptic  activity  of  such  a 
substance. 

Note.  —The  dyes  referred  to  belong  to  the  Monazo,  Disazo, 
Triphenyl-methane,  Xanthin,  Azin,  and  Thiazin  clas 

/'"'/<  '>'..)  The  investigations  of  Ehrlich  have  shown  that  basic  dyes  color  the  brain 
gray,  and,  moreover,  they  color  nerve  fiber  very  well,  and  are  therefore  to  be  regarded  as 
neurotropy  .  Thedyeacids,  on  the  other  hand,  do  not  dye  nerve  fiber,  and  in  particu- 
lar the  at)  itituted  sulphonic  acids  do  not  dye  tissue  at  all. 

ir>.  Meyer,  in  his  paper  on  "A  preliminary  communication  on  the 
toxicity  of  some  aniline,  dyes  tuffs"  (./.  Amer,  ( 'In  iii.  Soc.f  t907,  v.  29, 
p.  892 

(Page  898.)  "A  manufacturing  confectioner  of  this  city,  for  whom  I  made  examina- 
tion of  colors  used  by  him,  informs  mo  that  a   yellow  color  sold  as  Anraniin  has  such 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS.  61 

high  tinctorial  power  that  1  ounce  will  color  2,000  pounds  of  candy  to  the  highest  yel- 
low tint  required  in  his  business.  It  is  obvious  that  the  toxicity  of  such  a  body  would 
have  to  be  very  high  to  render  it  harmful  in  such  use."  Conclusions  of  this  kind  do 
not  take  into  account  the  possible  detrimental  action  ensuing  on  healthy  as  well  as 
diseased  persons  from  long-continued  use  of  small  quantities  of  foreign  substances. 

{Page  909.)  The  same  author  raises  objection  to  feeding  experiments  on  the  ground 
that  substances  are  thereby  introduced  greatly  in  excess  of  the  amounts  generally 
found  in  foods  and  that  the  ill  effects  "are  liable  to  be  due  to  the  excess  and  in  long- 
continued  experiments  due  to  a  cumulative  action  of  the  excess."  Surely  if  exc< 
amounts  have  a  cumulative  action,  small  amounts  may  also  finally  show  toxic  effects 
due  to  retention  and  accumulation  of  the  poison.  To  declare  a  substance  entirely 
innocuous  would  require  evidence  as  to  its  nontoxicity  both  to  normal  and  diseased 
persons  after  its  long-continued  administration  in  both  small  and  large  doses.  The 
most  extreme  contingencies  would  have  to  be  provided  for.  The  above  objections  to 
feeding  experiments  are  therefore  not  valid.  It  is  hoped  that  a  study  of  the  effects 
on  metabolism  of  some  of  these  substances  will  help  to  further  elucidate  the  subject. 

He  summarizes  the  results  of  his  physiological  investigations  of 
seven  different  coal-tar  colors  as  follows: 

1.  Several  commercial  organic  dyestuffs  (Curcumin  S,  Tartrazin,  Xaphthol  Red  8, 
Carmois  in  B,  Naphthol  Yellow  S,  Gold  Orange,  and  Ponceau  2  R)  were  studied  ae 
to  their  general  effects  on  dogs  when  administered  in  varying  amounts  and  during 
fairly  long  periods  (two  weeks). 

2.  None  of  these  dyestuffs  under  the  conditions  above  indicated  exhibited  any 
marked  degree  of  toxicity.  There  was  only  one  fatal  result,  which  may  have  been 
due  to  influence  independent  of  the  action  of  the  colorant. 

Similar  quotations  from  the  literature  could  be  added  to  the  fore- 
going! but  these  are  beyond  question  sufficient  to  show  that  a  wide 
divergence  of  opinion  as  to  the  harmless  or  harmful  nature  of  the 
coal-tar  colors  as  a  class  does  exist  among  scientific  men,  and  that  all 
those  above  quoted  agree  that  there  are  some  at  leasl  of  the  coal-tar 
colors  which  even  in  a  pure  state  may  be  harmful  to  human  health, 
and  that  the  question  of  actual  harmfulness  under  the  conditions 
of  actual  use  in  foods  and  the  consumption  of  foods  Is  regarded  by 
some  as  being  properly  ans'svered  in  the  negative  and  by  others  as 
being  properly  answered  in  the  affirmative.  The  question  of  amount 
of  color  employed  in  t  he  food  products  and  t  he  amounts  of  such  food 
normally  eaten  are  therefore  raised  by  some  as  the  deciding  factors. 

In  this  connection  the  following  statement  from  page  19  of  the 
arguments  before  the  Committee  on  Patents  in  the  Bouse  of  Repre- 
sentatives, April  8,  15,  16,22,29,  L908,  may  be  of  interest: 

*    *    *    It  should  lx-  remembered  thai  after  a  new  chemical  ha-  been  disc* 
and  patented  it  requirei  a-  many  u  three  year-  oi  experiment  before  we  dare  offer  it 
in  this  country  ai  a  medicine  for  human  beings.    These  experiments  are  cond 
ah  cud  before  we  receive  il  here,     li  is  first  tried  "n  animal-  and  gradually,  with 
caution,  extended  t>>  human  beings  in  tin-  foreign  hospitals,  -  certain  its 

physiological  effects  quantitatively  upon  the  various  organs,  both  when  i> 
an-  in  the  healthy  state  and  when  they  are  affected  by  various  disorders    *    *    *. 


62  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

A  search  of  the  literature  herein  compiled  fails  to  disclose  any  such 
searching  physiological  examination  of  any  of  the  coal-tar  colors 
recommended  for  use  by  human  beings  in  food  products,  as  is  asserted 
in  the  above  quotation  to  be  necessary  in  the  case  of  a  new  chemical 
intended  for  use  as  a  drug.  If  Fraenkel,  as  quoted  on  page  60,  is 
correct  in  his  statement  that  coal-tar  colors  act  physiologically 
because  they  are  chemicals  and  not  because  they  are  coloring  matters, 
then  coal-tar  coloring  matters  prior  to  use  in  foods,  in  winch  they  are 
used  by  the  young  and  the  old,  the  well  and  the  sick,  without  restric- 
tion and  without  supervision,  should  also  be  thoroughly  tested,  and 
very  few,  if  any,  coal-tar  colors  seem  to  have  been  examined  with 
the  thoroughness  set  forth  in  the  above  quotation.  That  uniformity 
and  purity  of  product  is  necessary  in  order  to  be  sure  that  the  chem- 
ical is  going  to  act  physiologically  in  the  same  way  every  time  is 
obvious.  According  to  Fraenkel,  what  is  true  of  a  chemical  is  just 
as  true  of  a  coal-tar  color,  and  if  uniformity  of  strength  and  cleanli- 
ness of  product  are  desirable  when  a  chemical  is  to  be  used  as  a  medi- 
cine, such  properties  are  equally  desirable  when  a  chemical  is  to  be 
used  as  an  ingredient  in  food. 

CLASSIFICATION   OF   OPINIONS    IN  LITERATURE   AND    IN   LEGAL 
ENACTMENTS  SHOWING  CONDITION  OF  THE  MARKET  IN  1907. 

The  literature  and  legal  enactments  hereinafter  grouped  under  the 
relevant  Green  Table  numbers  have  been  classified  as  (1)  unfavora- 
ble— i.  e.,  only  unfavorable  reports  found  in  the  literature;  (2)  favor- 
able, and  (3)  contradictory  reports,  as  each  case  required;  so  that 
under  each  Green  Table  entry  there  is  not  only  the  relevant  literature, 
but  also  the  character  assigned  to  it  for  the  purpose  of  coming  to  a 
conclusion  as  to  the  propriety  of  the  use  of  such  color  in  foods  as 
based  on  such  literature,  which  conclusion  formed  in  that  respect 
the  basis  for  Food  Inspection  Decisions  Nos.  76,  77,  and  106. 

However,  ii  does  not  follow  that  all  dyes  placed  in  the  "favorable'' 
list  are  actually  harmless;  the  investigations  or  opinions  reported  of 
each  may  very  well  be  based  upon  insufficient  data.  This  classifica- 
tion, therefore,  is  merely  intended  to  reflect  the  present  state  of  the 
literature  with  respect  thereto,  and  is  not  necessarily  final  nor  con- 
clusii  e. 

In  substantially  all  the  recorded  cases  the  observers  directly  or 
indirectly  asserl  the  absence  of  arsenic  and  mineral  poisons  in  the 
dyes  subjected  to  physiological  best,  but  the  kind  of  other  impurity, 
if  any,  is  not  stated. 

For  the  purpose  of  a  comprehensive  survey  of  the  literature  and 
Legal  enactments,  the  following  tabulation  is  presented: 


COMPILED   DATA   UXDER   GREEN    TABLE    NUMBERS. 


63 


Condition  of  the  United  States  color  market  in  the  summer  of  1907. 

[x=notoD  market.    Figures  indicate  number  of  dealers  offering  sample.    Cross  lines  separate  the  several 

groups.] 


Green 

Table 

number. 

Unfa- 
vor- 
able. 

Favor- 
able. 

Con- 
tradic- 
tory. 

Green 

Table 

number. 

Unfa- 
vor- 
able. 

Favor- 
able. 

Con- 
tradic- 
tory. 

Green 

Table 

number. 

Unfa- 
vor- 
able. 

Favor- 
able. 

Con- 
tradic- 
tory. 

1 

X 
X 

X 

X 

164 
166 
169 
188 
197 
201 
240 
269 
277 
287 

X 

521 

527 

X 
X 

2 

X 

1 

i " 

4 

3 

M 

10 

X 

530 
532 

X 
X 

5 

6 

2 

1 

...... 

563 

X 

8 
9 

5 

1 
2 
6 
2 

X 

X 

2 

1 

X 
X 

2 

X 

X 

572 
574 
576 

X 

X 

11 

1 

13 

X 

14 

394 
398 

X 

...... 

15 

584 
593 
599 
600 
601 

614 

1 

16 

X 
X 
X 

17 

399 

X 

18 
28 

X 

425 

3 

1 

41 

X 
X 

43 

427 
428 
433 
434 
435 
448 
450 
451 
457 
459 
462 
467 
477 
478 
479 
480 
483 
488,490 

2 
3 

55 

65 

2 

l" 

1 

620 
639 

X 

X 

70 

78 

X 

4 

...... 

X 

5 

X 

84 

2 

X 
X 

649 
650 
651 

.',.-,4 

X 

85 

2 

86 

X 
X 

87 

88 

X 

X 

X 

89 

"~6" 

1 

X 
X 

2 

X 
X 

659 

X 

92 
93 

887 

1 

94 
95 

2 

670 

675 

X 
X 

97 

1 

X 

102 

X 

6 

1 

"5" 

103 

X 

689 

105 
106 

107 

3 

502 
504 
512 
516 
517 
520 

2 

7 

5 

Totals 
106 
*50 

33 

82 
1  16 

...... 

3 

41 

138 

X 
X 
X 

160 

5 
2 





163 

1  Italicized  fijniros  are  colors  in  the  permitted  list,  Food  Inspection  Decision  7f>. 

2  On  United  States  market  In  1907. 

This  table  shows  thai  of  the  106  coal-tar  dyes  examined  physiolog- 
ically only  50  were  on  the  United  States  market;  Further,  out  of  33 

"  unfavorable"  dyes  S,  or  one-fourth,  were  on  the  United  States 
market;  out  of  32  "favorable"  dyes  L6,  or  one-half,  were  on  the 
United  States  market,  and  finally  thai  oul  of  41  "contradictory" 
dyes  20,  or  very  nearly  two-thirds,  were  on  the  United  States  market 
in  t  lie  summer  of  1 907. 

Aflfliirmng  this  classification  to  be  substantially  and  essentially  fair, 
the  only  Green  Table  numbers  which  are  of  interest  for  the  present 
discussion  are  those  classified  under  "favorable/1  because  any  color 
positively  injurious  or  of  doubtful  character  is  considered  as  being 
properly  excluded  from  use  in  food  products.  The  Green  numbers 
classified  as  •favorable"  are  32  in  number,  as  follow  5;  28; 

13;  102;  103;  106;  107;  L< 
jfS6;  W2;  467;  -177;  512;  617;  520;  521  ;  527;  576;  59 


64 


COAL-TAE  COLORS  USED  IN  FOOD  PRODUCTS. 


Of  these  32,  16  were  on  the  United  States  market  in  the  summer 
of  1907  and  their  composition  disclosed;  they  are  presented  in  the 
following  table,  together  with  the  number  of  dealers,  out  of  a  possible 
12,  offering  them  for  sale. 

Distribution  of  "favorable"  colors  on  the  American  market  in  1907. 


Gr^en 

Table 

number. 

Number 
of  dealers 
handling. 

Green 

Table 

number. 

Number 
of  dealer? 
handling. 

Green 

Table 

number. 

Number  1    Green 
of  dealers'!     Table 
handling,    number. 

Number 
of  dealers 
handling. 

4 

65 
85 
89 

10 
2 
2 

103 
105 
107 
169 

6 

1 
7 
1 

240 
433 
435 
462 

1 

1 

4 

■2 

512 
517 
520 
692 

3 
5 
2 

3 

From  among  these  16,  six  of  the  seven  permitted  colors  of  Food 
Inspection  Decision  No.  76  were  selected.  The  process  of  selection 
and  of  elimination  is  described  on  page  166. 

CLASSIFICATION    ACCORDING    TO    CHEMICAL    COMPOSITION    AND 

SUITABILITY. 

In  the  following  table  the  chemical  composition  of  the  substances 
corresponding  to  the  Green  Table  numbers  is  given,  and  their  classi- 
fication according  as  the  literature  is  regarded  as  being  (1)  unfavor- 
able, (2)  favorable,  or  (3)  contradictory  in  regard  to  the  color.  The 
colors  are  also  arranged  in  the  groups  to  winch  they  belong  chemically, 
so  that  this  table  shows:  (1)  The  number  of  groups  reported  on  in  the 
literature,  (2)  the  number  and  composition  of  members  of  each  group 
so  reported  on,  and  (3)  the  interpretation  here  placed  upon  such 
reports  in  literature.  This  table  is  given  in  the  expectation  that  it 
will  be  of  use  to  chemists  and  physiologists. 

Opinions  as  to  suitability,  classified  according  to  groups  and  chemical  composition. 
(The  chemical  nomenclature  is  that  of  the  Green  Tables;  "a"  is  used  for  alpha  and  ••  1>"  for  bete.) 


T'nfa'. 


Favorable. 


Contradictory. 


NITRO  COLORS. 

1.  Symmetrical  frinitrophenol. 

2,  Dinitro  o  and  p-eresol. 

.',.    Diiiilro-a-naphlhol. 

fc  Bexanltro-diphenylamliL 


Kfethyl-benzenyl-amldo-thlo- 

'.l-a/o-a-naphthol  <li- 

lonio  a  Id. 
94.  Benzene-azo-p]  razahme-oar* 

■di  tulpnonic  add. 
'M.  BnlphoHO-toluene-azo-b-  naph- 
tnoL 


4.  Dinitro-a-naphthol-b-mono- 

sulphonic  acid. 

5.  Diniiro-a-naplithol-a-  mono- 

sulphonic  acid. 


28,  p-nltro-benzene-azo-a-naph- 
thylamln  p-eulphonloacld. 

65.  a-naphthalene-aso-b-  naph* 

thol-dlsulphonlo  add, 
dphobeni  ene-aio-a* 

oaphthoL 
39.  p  -  nuphobensene  -  aio  -  dl  - 

phenylamm-eu  1 1> h onic 

add. 
22.  Wphenylamln  yellow  with 

iLitro-'liphriivlaiiuii. 


s.   Aiiihlo-a/D-binzi'iic-'li-  and 

monoeulpbonlo  add, 

2.    AmldO  -  MO  -  toluene  -  disul- 

pbonlo  add. 
1 1.  Bentcne aaO'b-paphthoi 

18.   Hen/i'iira/o-li-  naphthol  -  b  - 

BulpuoDk  add. 

1 1.  Benxene4tfo>b-aaphthol    dl- 
sulphonlc  acid  G. 


COMPILED  DATA  UNDER   GREEN   TABLE   NUMBERS.  65 

Opinions  as  to  suitability,  classified  according  to  groups  and  chemical  composition — Con. 


Unfavorable. 


mono  azo  colors— continued. 


DISAZO  COLORS. 

164.  Sulphobenzene-azo-sul  p  h  o  - 
benzene-azo-b-naphthol  - 
sulphonic  acid. 

201.  Hydrochlorid  of  toluene  dis- 
azo-m-tolylene-aiamin. 

277.  Ditolyl-disazo-binaphthion  i  c 


N1TROSO  COLORS. 

STTLBENE  COLORS. 

DIPHENYLMETHAXE  COLORS. 

4.'.',.  J I  ydrochlorld  of  lmido-tetra- 
methyl-diamido-diphenyl- 
methane. 

TRIPIIENYLMETIIANE  COLORS. 

434.  Dimethyl -dibenzyl-diarnido- 
trlphenyl-carbinol-tris  u  1- 
phoni 

4.V.t.  Chloric!  of  heptamethyl-rosan- 
ilin  chlond. 


478.  Triphenyl-pararosanilin     di- 
uri'l  trisulphonic  acid, 
tphenyl-pararosanilin-l  r  i- 
sulphonic  acid. 

488.490.  Hydrochlorid    of    phe- 
n>  1-t  •  Diethyl- 

triamido-diphenyki-aaph- 
thyl  carbinol. 


Favorable. 


93.  p-sulphobenzene-azo  -  dioxy- 
naphthalene  sulp  h  o  n  i  c 
acid. 

102.  p-sulpho-raphthalene  -  azo  - 

b-anphthol. 

103.  p-sulphonaphthalene-azo-a- 

naphthol-p-sulphonic  acid. 
105.  p-sulpho-naphthalene  -  azo  - 

b-napbthol  monosul- 

phonic  acid. 
107.  p-sulpho-naphthalene  -  azo  - 

b-naphthol-dis  u  1  p  h  o  n  ic 

acid. 


166.  Sulphobenzene  -  azo-sulpho- 
benzene  -  azo  -  p  -  tolyl  -  b- 
naphthylamin. 

169.  Sulphotoluene-azo-foluene- 
azo  -  b  -  naphthol  -  a  -  sul- 
phonic acid. 

240.  Diphenyl  -  disazo  -  binaph  - 
thionic  acid. 


Contradictory. 


394.  Dlnitroso-resorclnol. 


399.  Azoxy-stilbene-di-sulphonic 
acid. 


433.  Diethyl- dlbenzyl-diamido- 
trlphenyl  carbinoi-disui- 
phonic  ;k  - 1  <  1 . 

).;.",.  Iu.-thvl-ditH-nzyl-diamido- 
triplionyl-carbinol-tris  u  1- 
phonicacid. 

sulphonic  acid  of 
lin  and  pararosanilin. 

■177.  Trlphfinyf- rowan  H  In 

aulphonJo  acid  and  trlphe- 
ii>  1  -  pararosanilin  -mono- 
iulpnonio  acid. 

4».7.  Dlsulphonicacld  of  dimethyl 
dibensyldi-ethy]  trianudo 
triphehylcarbiuol. 


15.  Benzene-azo-b-naphthol     di- 

sulphonic  acid  R. 

16.  Dimethyl-amido  -  azo  -  ben- 

zene. 

17.  Hydrochlorid  of  diamido-azo- 

"benzene. 

18.  Hydrochlorid  of  benzene-azo- 

m-tolvlene-diamin. 

41.  Hydrochlorid  of  toluene-azo- 
m-tolylene-diamin. 

43.  Toluene-azo-b-naphthol- sul- 
phonic acid. 

55.  Xylene-azo-b-naphthol-disul- 
phonic  acid. 

70.  Dichloro-phenol-azo-b  -  naph- 
thol. 

84.  p-sulphobenzene-azo  -  resorci- 
nol. 

86.  p-sulphobenzene-azo-  b-naph- 

thol. 

87.  p-sulphobenzene-azo-dimeth- 

ylanihn. 

88.  p-sulphobenzene-azo  -  diphe- 

nylanun. 
95.  m-sulphobenzene  -  azo-diphe- 

nylamin. 
106.  p-sulphonaphthalene  -  azo-b- 
naphthol-disulphonic  acid. 

138.  Blsulphobenzene  -  disazo  -  a- 

naphthol. 
160.  Sulphobenzene-azo-benzene  - 

azo  -  b  -  naphthol  -  niono- 

sulphonic  acid. 
163.  Sulphobenzene- azo -sulpho- 

benzene-azo-b-naphthol. 
188.  Disulpho-b-naphthalene-azo- 

a-naphthalene  -  azo  -  b  - 

naphthol-disulphonic  acid. 
197.  Hydrochlorid  of  benzene-dis- 

azo-phenylene-diamin. 
269.  Ditolyl  -  disazo  -  bi  -  salicylic 

acid. 
287.  Ditolyl-disazo-bi-a-  naphthol- 

p-siilphonic  acid. 

:  108.  N  It  roso-b-napht  hol-b  -  mono  - 
sulphonic  acid. 


427.  Chlorid  of  tetra-methyl  di-p- 

Idc-triphenyl-carbinoi. 

428.  Sulphate  or  chlorid  of  tetra- 

eihyl-diainido- trip!. 
LnoL 
44s.  Hydrochlorid  i  i 

Janilln   and 
in. 
4.v.  llydrochlorids  or  a 

inoiio-di  or  trlmethyl  (or 
ethyl)  rosaolUna  and  para- 

'.  ims. 
451.  Hydrochlorid  Of 

ollin. 
4.".7.    Hydrochlorid.    snip' 

triphenyl  i 
lm  and  triphenyl  pararoa- 
anilin. 

1-rosantlin  and   (ri- 
. nilin     sul- 

,- 

rin 

kCid. 


97291°— Bull.  147- 


66  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

Opinions  as  to  suitability,  classified  according  to  groups  and  chemical  composition — Con. 


Unfavorable. 


Favorable. 


Contradictory. 


XANTHENE    COLORS. 

502.  Triethylrhodamin. 
516.  Diiodo  fluorescein. 


ACRIDIN   COLORS. 

530.  Ilydrochloridofdiamido-phe- 

"  nvl-dimethyl-acridin. 
532.  Nitrate    of  chrysanilin    and 
homologues. 

ANTHRACENE   COLORS. 


INDOPHENOL  COLORS. 

572.  Tin  compound  of  dimethyl 
p-amido  phenyl-p-oxy- 
a-naphthylamin. 

571.  Ilydrochlorids  of  p-pheny- 
lene-diamin-p-amidophe  - 
nol  and  diamido-dipheny- 
lamin. 

AZIN  COLORS. 

602.   Spirit  Nigrosines. 

014.  Ainido-  naphthyl- naphtha  - 
zonium  chlorid  and  dia- 
mido  naphthyl-naphtha- 
zonium  chlorid. 

ox  AZIN  COLORS. 

020.  Dimethylamido  -  dioxy  -  phe- 
nazoxonium  carboxylate. 

G39.  Chlorid  of  dimethyl-amido- 
naphtho  -  phenoxazonium 
chlorid. 

TIUAZIN  COLORS. 

640.  Zinc -double -chlorid  of  di- 
methyl -  diamido-phenaz- 
th  ionium  chlorid. 

B61.  Nitromethylene  Blue. 

664.  chlorid  of  dimethyldiamido- 
toluphenazthionium. 

TmOBKKZZKTL  COLORS. 

669.  I ><'liydrothiotoluidin. 

quoroun  colobs. 

•/uinophthalone. 

670.  Sulphohydro  derivative  of  a 

polytnladn. 
675.  Tmocateohlrj  S  (composition 
unknown). 

DTDIOO  <  oi.oits. 


512.  Tetrabromofluorescein. 

517.  Tetraiodofluorescein. 

520.  Tetraiododichlorofluorescein. 

521.  Tetrabromotetrachloro  fluor- 

escein. 
527.  Sodium     bisulphite      com- 
pound ofccrrulein. 


504.  Hydrochlorid    of  diethyl-m- 
amido-phenol-phthalein. 


570.  New  Cray  (composition  un- 
known). 


.-.03. 


000. 


Phenyl-  and  tolyl-safranins. 

Mixtures  of  diariilido-amido- 
trianilido-,  and  tetraani- 
lido  -  phenyl  -  phenazo  - 
nium  chlorids. 

Indulins  and  fluorindins. 


692.  IndiRotln  disulphonio  acid. 


563.  Dioxy-anthraquinone-b-qui- 
noiin. 


584.  Diamidophenyl     and     tolyl- 

tolazonium  chlorids. 
001.  Sulphonated  indulins. 


050.  Chlorid     of     tetramethyl-di- 
amido-phenazthionium. 


680.  ImliRotin. 


COMPILED   DATA   UXDER   GREEX    TABLE    NUMBERS. 


67 


PHYSIOLOGICAL  ACTION  OF  COAL-TAR  DYES. 


SUMMARY    OF    SYMPTOMS. 


A  rough  summary  of  the  symptoms  noted  or  positively  deter- 
mined to  be  absent,  the  number  of  the  deaths  produced,  and  the 
number  of  cases  in  which  nothing  abnormal  was  noticed  may  serve 
as  a  convenient  guide  in  considering  the  detailed  statements  herein- 
after given  relative  to  all  the  symptoms,  clinical  data,  legislative  and 
other  publications,  or  permissions. 

In  the  following  tables  are  brought  together  most,  if  not  all,  of  the 
recorded  observations  with  respect  to  the  humans  and  other  animals 
upon  which  the  physiological  action  of  coal-tar  dyes  has  been  studied 
as  well  as  the  results  of  autopsies  when  recorded.  The  columns 
headed  " Unfavorable,"  " Favorable,"  and  " Contradictory"  have  the 
same  significance  as  in  the  preceding  table;  italicized  numbers 
are  those  of  the  permitted  colors  of  Food  Inspection  Decision  No.  76. 
Asterisked  numbers  indicate  that  the  dye  was  administered 
hy  podermically . 

Experiments  on  Do«.- 

Table  I. — Observations  on  dogs. 
(Reference  to  Green  Table  numbers.) 


Symptoms. 

Unfavorable. 

Favorable.                          Contradictory. 

Deaths 

1;  2: 3;  488  or  490;  574;  639 
(2);  649. 

3;  488  or  490 ;  572;  57 

16  (2);  55;  7(>v 

Autopsies 

108;  105;300;467;  K 

188»; 
480*;  801;  I 

• 

Stained  skin 

639;  649. 
1 

Stained  conjunctiva' 

Respiration  difficulties 

Temperature  normal 

Temperature  hi^h 

Temperature  low 

Genera]  depression 

Weakness 

1 

1;  a 

2;  620;  649 

407 

461;  601. 

488  or  490;  3 

188  or  490 

4.M. 

426;  t.49;  07.") 

66a 

I;  3;  fl                    

1'.;  488. 

Loss  of  weight 

1:  488  W  190;  8    ' 

17;  18;  4                 •  I;  65a 

Emaciation. . 



Loss  of  appetite 



ti50. 

Colore. 1  urine 



l;  502; 
516; 
861;  0 

621;  1 

L;  18;  it:  16; 

I  rine  not  affected 



l;  8;  . 





601. 

Albuminuria.   . 

Albuminuria  doubtful 

Alkaline  urine 



28;  166;  240 

I 

L;  17,  18,  or  11:  70; 

• 



Bladder  Irritation 

Thirsl 



Thin  stool 

Diarrhea 

Blood}  stool. 

68  COAL-TAR    COLORS   USED   IX    FOOD   PRODUCTS. 

Table  I. — Observations  on  dogs — Continued. 


Symptoms. 

Unfavorable. 

Favorable. 

Contradictory. 

Pus  in  stool ' 

650 

Stool  desires 

502 

Vomiting 

Retching 

1;  2;  3;  6;  97;  27" 
488or490;51( 
614;  639;  649 

675 

1  488  or  490;  639; 
488  or  490;  639. 

;42S 

>;532 
670 

649; 

;479; 
;574; 
675. 

675... 

399; 

*•• 

433; 

467 

576;  692... 

11;  16;  86;  87;  95;  197;  269; 
428;  448;  451;  483;  650. 

16;  86. 

Salivation 

584. 

Anemia 

Stupor 

601. 

Desire  to  sleep 

451. 

Catarrh  of  eves  and  nose . . 

451. 

Cramps 

1;  2 

601. 

Convulsions 

2;  675 

Tremors 

87. 

Congestion 

Paralysis  of  limbs 

649 

1;  675 

16;  55;  87;  428;  450. 

Destroys  coloring  matter 
of  blood. 

1;  2 

87;  601. 

601. 

650. 

i 

The  following  table  discloses  the  results  of  the  autopsies  made  and 
reported  on  dogs. 

Table  II. — Autopsies  on  dogs. 


Symptoms. 

Unfavorable. 

Favorable. 

Contradictory. 

No    change    in    internal 
organs. 

87. 

105;  399;  467;  477;  593 

103 

87  III;  457. 

No  change  except  whole 
interior  colored  red. 

LTVER. 

Fatty  degeneration 

572;  620;  639 

601;  650. 

488  or  490...                               

451  (2);  480  II*;  601. 

Pale.. 



451  (2). 

574 

649 

650. 

Blood-Oiled  . 

574 

KIDNEYS. 

3;  639;  649 

451  (2);  480*  (II). 

Filled  with  decomposed 
blood  corpuscles. 

639 

451  (2). 

480  (1);  601;  650. 

Soft. 

480*  11. 

488  or  490  .. 

601. 

Blood-filled 

574 

620;  639 

692 

1    IIC'l 

650. 

650. 

STOMACH. 

488  or  490 

650. 

Catarrh 

188  oi 

650. 

;  0 

801. 

with  colored  inw 
l.t  \ 
Filled  with  blood 



:,:  i            

601. 

■BAST. 

574 

Paraly*                  



16  (2);  87  I;  428;  87  II. 

COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS.  69 

Table  II. — Autopsies  on  dogs — Continued. 


Symptoms. 

Unfavorable. 

Favorable. 

Contradictory. 

INTESTIN'ES. 

Colored 

488  or  490 

650. 

Catarrh 

488  or  490 

COLORED. 

Brain 

650. 

Fat 

650. 

Skin 

650. 

Pleura 

Heart  sac 

650. 

Diaphragm 

650. 

488  or  490 

650. 

480*11. 

All  organs  swollen 

480*11. 

General  congestion 

Peritonitis 

3(11) 

70*. 

Fat  all  disappeared 

Flabby  muscles 

G39 

639 

In  this  connection  it  may  be  of  interest  to  note  that  out  of  16  dyes 
producing  death  when  administered  through  the  mouth  to  dogs,  7 
were  on  the  United  States  market  in  the  summer  of  1907.  Their 
Green  Table  numbers  are  as  follows,  the  numbers  in  parentheses 
indicating  the  number  of  makers  or  importers,  out  of  a  possible  12: 
offering  them:  55  (2) ;  86  (8) ;  95  (2) ;  428  (3) ;  451  (5) ;  601  (1) ;  650  (2). 

The  following  table  gives  the  Green  Table  numbers  of  coal-tar  dyes 
which  on  administration  to  dogs  positively  did  not  in  certain  specific 
cases  produce  the  particular  disturbances  recited,  although  the  case  of 
the  several  colors  as  a  whole  is  regarded  in  the  literature  as  ■■favor- 
able," " unfavorable,"  or  "contradictory,"  as  stated. 

Table  III. — Observations  on  dogs  showing  definite  negative  result*  in   specific 
grouped  under  the  general  verdict  of  the  literature  as  a  wholt . 


Symptoms. 

Unfavorable. 

Favorable. 

Contradictory. 

014 

4:  105;  462 

K;  601. 

I  >i  irrlnM 



03;  106:  -\  ■ 
521;  527;  576. 

; 

Allmminiirhi 

6;  97;  277;   i 
051;  659. 

14;  16; 
197;                         801. 

1  i92 

That  is,  when  these  dyes  were  tried  od  dogs  the  observers  reported 

in  certain  specified  cases  positively  and  definitely,  the  absence  of  any 

of  the  symptoms  named. 

It  is  stated  of  the  follow  ing  colors  that  they  produced  no  bad  effects 
in  certain  specified  cases:  \; 9;  55;  B6j  105;  L88;  L97;  240;  157;  572; 

593.      No    had    effect    except    colored   urine:     13,  95.      Nb  had   effect 

except  albuminuria:  88,287.     N<>  bad  effect  except  loss  of  weight: 

12.5  pei- cent   (17.   is,  or  41). 

It  is  therefore  t  rue  of  all  of  these  coal-tar  d\  e>  that  then'  are  Condi- 
tions under  which   they   have  0660  oh^erved   not    to   produce  the  had 


70 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 


effects  as  above  set  forth;  but  this  tabulation  must  not  be  taken  to 
mean  that  these  dyes  can  not,  under  any  conditions  whatever,  produce 
untoward  results ;  the  reverse  is  true  in  most  cases. 

Experiments  on  Human  Beings. 

The  Green  Table  numbers  of  those  colors  concerning  which  experi- 
mental data  are  available  on  humans  are  as  follows :  1 ;  2 ;  3 ;  4;  6 ; 
9;  (17,  18,41);  55;  65;  85;  86;  95;  102;  103;  105;  106;  107;  197; 
427;  428;  448;  462;  532;  602;  650. 

The  symptoms  produced  are  classified  in  the  following  list: 

Internally  administered. 


Not  poisonous 4; 

9;   55;   65;   85;  95;   102; 

103; 105; 106; 107; 448; 462 

Poor  general  condition 86;  650 

Fever 2 

Loss  of  appetite 2 

Vomiting 3;  532;  650 

Intestinal  irritant 650 

Diarrhea 532;  650 

Bladder  irritant 650 

Colored  urine 86;  95;  650 

Albuminuria 650 

Increased  micturition 650 

Irritant 532 

Inflammation 532 


Bad  taste  in  mouth 86 

Restlessness 86 

Rush  of  blood  to  head 86 

Vertigo 86;  650 

Headache 650 

Delirium 650 

Twitching  of  muscles 650 

Yellow  coloration  of  skin 3 

Yellow-colored  mucous  membrane.  3 
Food  colored  with  it  made  a  family 

sick 3 

Adults  withstand 1 

Children  and  weak  adults  do  not 

withstand 1 

Deaths 2;  3 

Autopsy l  3 


Dryness  of  throat 86 

It  should  be  noted  that  of  the  13  dyes  here  classed  as  not  poisonous 
to  humans  all  but  No.  102  were  on  the  United  States  market  in  the 
summer  of  1907,  as  is  shown  in  the  following  table: 


Number  of  dealers  offering  these  nonpoisonous  colors  in 


1907. 


Green 
Table 

numbers. 

Sources 
offering 

same. 

Green 

Table 

numbers. 

Sources 

offering 

same. 

Green 

Table 

numbers. 

Sources 
offering 

same. 

Green 

Table 
numbers. 

Sources 
offering 

same. 

9 
55 

,0 

1 

2 

i  85 

i| 

103 
id;, 
106 

(i 
1 
5 

107 
448 
463 

7 
4 
2 

1  On  permitted  list,  Food  inspection  Decision  76. 
Symptoms  produced  by  external  application  of  certain  colors  (Green  Table  nurnbett). 


I  dermatitis 4 

Eczema (17,  18,  or  41);  197;  602 

Inflammation 427;  428 


Burning 2;  427;  428 

Itching 2;  6;  427;  428 

Blister* 2;  6 

Swelling 427;  428 

It  should  be  noted  thai  No.  86  Ims  been  tried  on  humana  and  has 
been  found  aot  to  produce  diarrhea  <>r  vomiting. 


1  Bemorrnagic  gastritis. 


COMPILED   DATA   UNDER   GREEN    TABLE   NUMBERS.  71 

G.  T.  3  has  apparently  killed  a  human  at  60  mg  per  kilo  and  the 
autopsy  disclosed  hemorrhagic  gastritis.  G.  T.  448  has  been  sug- 
gested as  a  possible  remedy  for  Blight's  disease.  It  should  also  be 
borne  in  mind  that  adults  can  stand  G.  T.  1  in  doses  of  540  to  900  mg 
daily  for  a  long  time,  whereas  children  and  weak  adults  stand  that 
substance  only  poorly. 

Experiments  ox  Small  Animals. 

Results  of  experimenting  on  rabbits  with  10  coal-tar  dyes  whose 
Green  Table  numbers  are  1,  2,  86,  89,  107,  427,  448,  504,  517,  and 
563  have  been  tabulated  as  follows : 

Paralysis 427* 

Cramps 427* 

No  harm  produced.  B9;  107;  44S;  504;  517 


Death 

Diarrhea 

....   1;  2;  427*;  563* 
1 

Colored  urine 

86 

Softened  feces 

86 

In  the  case  of  the  numbers  marked  with  an  asterisk  the  color 
administered  hypodermically.     In  this  connection  reference  should 
also  be  had  to  the  paper  of  Penzoldt  abstracted  in  Section  VIII, 
page  55. 

The  four  coal-tar  dyes  55,  103,  425,  and  480  have  been  tested  on 
guinea  pigs  and  no  disturbance  was  noticed  in  all,  but  hi  the  case  of 
103  occasional  thirstiness  was  observed.  Xo.  448  has  been  fed  to 
hens  without  damage,  and  Xo.  2  has  been  recommended  as  an  insect- 
icide, a  fungicide,  and  a  mouse  poison. 

GENERAL    STATEMENTS. 

The  following  statements  may  be  of  interest  before  the  detailed 
compilation  is  read: 

1.  O.  Buss   (Forschungsber.   iiber   Lebensmitttl,    1896,    vol.    2,    j>j>. 
163-197,  237),  in  a  paper  entitled  " Contributions  to  the  Spectrum 
Analysis  of  some  Toxic  and  Pharmacognostically  Important  Coloring 
Matters,  with  Special  Consideration  to  the  l'ltra-\ "inlet ."  cites 
poisonous  the  following  (Green  Table  numbers  follow  in  parent 
wherever  connection  could  be  satisfactorily  established): 


Picric  Acid (1) 

Dinitroo-  and  p-Greeol (2) 

Martina  Yell  m (3) 

Aurantia (6) 

Fast  Yell,  m (8) 

Orange  II (86) 

As  nonpoisonous: 
Naphtfaol  Yellow (4) 

Eoain 

Erythremia 

Anilin  Blue 

As  doubtful: 


Metaail  Yellow 

Oorallin 

Stiraniii 

Methylene  Blue 

[odin  Green 

AUsarin  Bl 

Naphthol  Green 

Malachite  Green 

Dahlia (450, 


Methyl  Violet (451,464)  |   Veeuvin 


72 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


On  the  following  Buss  is  noncommittal: 


Auramin (4-5) 

Biebrich  Scarlet (163) 

Water  blue (480) 


Magenta (448) 

Aurin J(483) 

Acid  Green (435) 


Naphthol  Black  of  various  brands,  which  seemed  to  be  mixtures. 

2.  It  has  been  pointed  out  that  the  following  nine  colors  are  harm- 
less: 


Naphthol  Yellow (4) 

Naphthol  Brown (?) 

Chinolin  Yellow (667) 

Pyrotin  RRO (115) 

Acid  Green (434, 435) 


Wine  Green (?) 

Milling  Red (?) 

Azo-acid  Blue (36) 

Fastrose (?) 


Most  of  these  have  not  been  examined  experimentally,  but  scien- 
tific studies  have  been  made  of  the  poisonous  qualities  of  Azo-Blue 
and  Naphthol  Yellow.     (Zts.  angew.  Chemie,  1896,  p.  21^.) 

3.  Chlopin  in  Ins  monograph  (see  p.  75)  says: 

On  the  basis  of  my  personal  experience  I  consider  the  testing  of  the  action  of  coal- 
tar  dyes  on  man  not  permissible,  since  such  experiments  may  induce  in  the  subjects 
of  experiment  more  or  less  serious  symptoms  of  poisoning,  for  which  in  some  cases 
there  are  no  antidotes  at  our  disposal.  To  such  accidents,  in  my  opinion,  only  the 
experimenter  himself  may  subject  himself,  because  he  knows  what  he  is  doing.  Pre- 
liminary tests  of  dyes  on  dogs  and  other  animals  afford  no  guaranty  of  escape  from  dis- 
agreeable accidents  which  may  take  place  in  the  testing  of  the  dye  on  man.     {Page  111.) 

These  data  and  calculations  convincingly  prove  how  erroneous  the  current  opinion 
is  that  for  the  coloring  of  food  substances  and  beverages  only  exceedingly  small, 
almost  unweighable,  quantities  of  dyes  are  used.     {Page  113.) 

On  page  221  et  seq.,  the  following  general  discussion  of  tins  subject 
is  found: 

The  Manner  of  Action  of  Poisonous  Dyes  on  the  Animal  Organism. 

The  mechanism  and  the  chemistry  of  the  action  of  the  artificial  dyes  of  the  aromatic 
series  on  the  animal  organism  remains  to  the  present  day,  with  few  exceptions, 
exceedingly  slightly  and  superficially  studied.  The  same  can  be  said  also  concern- 
ing the  pathological  and  anatomical  changes  which  are  induced  by  these  dyes. 

More  than  the  others  there  have  been  studied  in  the  toxicological  respect  the  dyes 
belonging  to  the  Nitro  group;  Picric  Acid;  Martius  Yellow  (Dinitro-naphthol  potas- 
sium), and  Saffron  substitute  (Dinitrocreeol  potassium.) 

According  to  Kobert,  these  dyee  belong  to  the  poisons  acting  on  the  blood.  Accord- 
ing to  tli'i  same  authority,  Methylene  Blue,  which  belongs  to  the  other  chemical 
group  of  Thiazins,  acts  similarly . 

In  the  fundamental  works  od  the  sanitary  investigation!  for  the  dyes,  by  Cazeneuve 
and    Lupine,  by  Weyl,  and  by  Bantori,   We  find  almost,  no  material  relating  to  the 

explanation  of  the  manner  <>i  tin'  action  oi  the  dyes.  These  Investigators  limiting 
themselves  to  a  very  cursory  description  of  the  symptoms  of  poisoning,  and  reciting 
in  most  general  terms  the  results  <>f  autopsy,  not  ei  en  indicating  the  cause  oi  death. 
Such,  for  instance,  are  the  reporti  of  autopsies  made  by  T.  Weyl  and  wmo  other 
invest  Igator  ,  a  -  quoted  aboi  e. 


J  Apparmtly  B  purified  formol  Corallin. 


COMPILED   DATA   UNDER   GKEEX    TABLE    XUMBEES.  73 

We  may  expect  that  more  detailed  investigations  in  this  respect  will  be  made  at  the 
proper  time  by  pharmacologists,  since  study  of  the  mechanism  and  chemistry  of  the 
action  of  the  poisonous  substances  on  the  animal  organism  is  their  province;  for  the 
hygienist  it  is  quite  sufficient  merely  to  establish  the  fact  that  a  given  substance  is 
poisonous  or  harmful,  and  he  need  not  go  any  further.  For  this  reason,  in  those  cases 
in  which  I  desired  to  clear  up  the  causes  of  death  of  the  animals  in  my  experiments, 
and  to  record  pathological  and  anatomical  changes  (although  by  the  terms  of  the  regu- 
lations governing  this  competition,  a  close  study  of  the  action  of  the  dyes,  and  the 
ascertainment  of  the  mechanism  and  chemistry  of  their  action  was  not  required),  I 
called  in  a  person  more  competent  than  myself  on  these  questions. 

Not  counting  the  duplicates  we  made  five  autopsies  all  told.     In  all  these  cases  death 
resulted  from  paralysis  of  the  heart.     The  pathological  and  anatomical  changes  in  all 
cases,  except  one,  did  not  present  anything  specific,  and  finally  reduced  themsel 
a  feebly  expressed  turbid  swelling  of  the  heart  and  of  the  liver,  a  rush  of  blood  to  the 
stomach,  and  a  congestion  of  the  internal  organs. 

The  exception  was  the  autopsy  of  a  dog,  which  died  from  Methyl  Orange;  this  dog 
died  with  the  symptoms  of  paralysis  of  a  cerebro-spinal  nature.  This  experiment  was 
made  twice,  and  the  autopsies  of  both  animals  showed  hyperemia  in  the  lowest  part 
of  the  spinal  column,  on  the  border  of  the  anterior  and  the  lateral  columns. 

As  to  the  symptoms  of  poisoning  not  resulting  in  acute  death,  here  most  frequently 
was  observed  vomiting,  diarrhea,  and  albumen  in  the  urine,  showing  disturbance  of 
the  functions  of  the  digestive  tract,  and  an  affection  of  the  kidneys. 

A  highly  typical  picture  of  poisoning  is  presented  by  the  sulphid  Vidal  dyes.  They 
cause  rapid,  almost  instantaneous,  deafening  of  the  animal,  whereupon  the  animal  falls 
on  one  side  in  convulsions  and  lies,  not  moving  its  body,  but  convulsively  and  rapidly 
twitching  its  anterior  limbs  during  several  minutes.  The  tongue  hangs  out  of  the 
mouth,  a  strong  secretion  of  saliva  is  noted,  then  vomiting  begins,  and  the  dog  gradu- 
ally begins  to  revive;  with  difficulty  he  arises  on  his  front  feet  and  sits  down,  not  being 
able  yet  to  stand  on  his  posterior  extremity,  which  is  in  a  state  of  paresis.  After  a  few 
hours  the  dog  becomes  normal.  The  symptoms  of  poisoning,  just  described,  are  exceed- 
ingly similar  to  the  supposed  "apoplectic  form"  of  poisoning  by  hydrogen  sulphid, 
which  had  been  studied  on  animals  by  K.  Lehmann,  and  which  was  observed  in  per- 
sons who  inhaled  air  containing  a  few  per  cent  of  this  gas.  Air  containing  0.1  to  0.3 
per  cent  of  hydrogen  sulphid  kills  cats  and  dogs  in  10  minute-. 

In  OUT  experiments  in  which  were  introduced  substances  containing  sodium  sulphid, 
the  poisoning  must  have  been  caused  by  hydrogen  sulphid  which  was  liberated  from 
the  dye  by  the  acid  of  the  gastric  juice,  and  which  could  cause  poisoning  also  through 
the  stomach  and  through  the  respiratory  apparatus. 

Fortunately  Vidal  dyes,  owing  to  their  repulsive  odor,  will  scarcely  find  a  wide 
application  in  coloring  food  and  beveragi 

Some  Reflections  R  eg  a  b  him.  IVihiii  i:  in  VK8TIGATXONS  OF  Dybs  FROM  ▲  Sani  iaky 

S  iw  DPOINT. 

The  present  investigation,  as  well  ai  all  the  investigations  oi  the  action  of  dyes  on 
animal-  by  previous  investigators,  had  for  its  object  the  solution  of  the  question  in 
what  number  there  exists  among  the  dyei  of  the  aromatic  .-  -v\<-<  dyes  which  possess 
pwi-.ip.u-,  or  more  or  l<  ■  pronounced  harmful  properties  (answering  essentially  the 
sanitary  toxicologi<  al  question).  Prom  the  practical  point  of  view  such  investigations 
presented  and  do  present  the  most  important  interest,  inasmuch  as  they  afford  a  possi- 
bility of  protecting  the  public  from  the  use  oi  obvious)  11  and  harmful  sub- 
stances, but  by  such  investigations  question!  iingly  sanitary  importance  are 
not  answered,  namely: 

1.  Ought  we  to  consider  as  quite  harmless  those  dyes  vrhich  do  not  induce  pro- 
nounced symptoms  o!  poisoning  and  which  are  designated  herein  l>v  the  term  nan- 
poisonous? 


74  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

2.  Is  the  usual  answer  which  is  given  to  the  hygienist  by  the  defenders  of  the  unre- 
stricted use  of  the  coal-tar  dyes  for  coloring  food  products  and  beverages,  namely,  that 
in  practice  the  dyes  are  introduced  into  the  human  organism  in  so  small  quantities 
that  their  properties  can  be  neglected,  justified? 

To  both  questions,  besides  the  facts  and  considerations  which  I  gave  above  in  my 
investigations,  we  may  reply  experimentally  in  two  ways: 

(a)  By  prolonged  investigations  continued  over  a  period  of  years  of  the  action  of 
very  minute  quantities  on  the  animal  organism,  which  has  so  far,  owing  to  the  incon- 
veniences of  such  long  experiments,  not  been  done  by  anybody;  and 

(6)  By  investigation  of  the  action  of  small  doses  of  dye  on  some  physiological  func- 
tions, and  first  of  all  on  the  activity  of  the  digestive  organs,  which  is  first  of  all  dis- 
turbed upon  the  introduction  of  dyes  into  foods  and  beverages.  The  solution  of  the 
last  question  can  be  best  promoted,  in  my  opinion,  by  experiments  made  on  dogs  and 
by  exploratory  examination  of  the  body  according  to  the  method  of  Prof.  Pawlow. 
Unfortunately,  experiments  such  as  these,  owing  to  the  difficulty  of  the  Heidenhain- 
Pawlow  operation,  are  inaccessible  to  the  majority  of  investigators. 

As  a  very  useful  substitute  of  such  investigations  may  serve  observations  on  the 
action  of  dyes  on  the  activity  of  the  digestive  juices  outside  the  body  of  animals. 

On  my  proposition  Dr.  A.  E.  Winogradow  began  in  my  laboratory  experiments  on 
the  action  of  small  doses  of  dyes  of  the  aromatic  series  on  the  digestion  in  vitro.  Dr. 
Winogradow  so  far  examined  25  coal-tar  dyes  in  this  respect  according  to  the  method  of 
Metta  and  convincingly  proved  that  in  insignificant  doses  coal-tar  dyes  (from  one-half 
to  4  milligrams)  entirely  stopped  the  digestion  of  albumen  by  artificial  gastric  juice. 
It  was  found  that  the  capacity  to  depress  the  digestion  is  possessed  not  only  by  poison- 
ous dyes,  but  also  by  dyes  which  proved  in  my  experiments  on  animals  nonpoisonous. 

It  is  quite  possible,  therefore,  that  an  admixture  of  coal-tar  dyes  will  exert  an  unfa- 
vorable influence  on  the  digestion  and  assimilation  of  food  prepared  from  products  col- 
ored by  them.  Experimental  proof  of  the  last  supposition  can  be  given  only  by  experi- 
ments on  the  influence  of  dyes  on  the  metabolism  of  substances  in  animals  and  man. 

COMPLETE  DETAILED  STATEMENT  OF  ALL  COMBINED  DATA. 
ABBREVIATIONS    OF   AUTHORITIES    CITED. 

The  data  hereinafter  given  is  brought  together  as  nearly  as  pos- 
sible under  the  Green  Table  numbers  to  which  it  is  pertinent.  It  is 
believed  that  the  literature  has  been  quite  thoroughly  searched,  and 
that  nothing  of  substantial  importance  has  escaped  recording  in  this 
compilation;  certainly  whatever  may  have  escaped  can  hardly  serve 
to  change  the  general  conclusion  to  which  this  compilation  leads. 

In  order  to  avoid  repetition  in  the  following  tabulation,  "Weyl" 
is  to  be  understood  as  referring  to  the  book  entitled  "The  Coal  Tar 
Colors,  with  Especial  Reference  to  their  Injurious  Qualities,  etc.,"  by 
Theodor  Weyl,  translated  by  Leffmann  and  published  in  Philadel- 
phia, Pa.,  in  L892. 

"Iieber"  refers  to  the  book  entitled  "The  Use  of  Coal  Tar  Colors 
in  Food  Products,"  by  Ilu.Lr<>  Ldeber,  published  in  New  York  in  1904. 

"Fraenkel"  refers  to  the  book  entitled  "Arzneimittel  Synthese," 
by  Dr.  Sigmund  Fraenkel,  published  in  Berlin  in  1900. 

"Confectioners  List"  refers  to  the  Official  Circular  from  the  Exec- 
utive Committee  of  tlnv  National  Confectioners'  Association  of  the 


COMPILED  DATA   UNDER  GREEN   TABLE    NUMBERS.  75 

United  States  entitled  " Colors  in  Confectionery"  and  reprinted,  in 
part,  in  the  book  entitled  "Food  Inspection  and  Analysis,"  by  Albert 
E.  Leach,  published  in  Xew  York  in  1906,  pages  630-634. 

" Resolutions  of  Swiss  Analytical  Chemists"  refers  to  these  reso- 
lutions as  published  in  Zeitschrift  fur  Xahrungsmittel  Untersuchung 
und  Hygiene,  1891,  page  293. 

"Schacherl"  refers  to  SchacherFs  publication  entitled  "Die  Zulaes- 
sigkeit  Kuenstlicher  Farbstoffe  zum  Farben  von  Lebensmitteln," 
published  in  Vol.  Ill,  pages  1041-1048,  of  the  Report  of  the  Fifth 
International  Congress  of  Applied  Chemistry  held  in  Berlin  June  2 
to  8,  1903. 

"Chlopin"  refers  to  Chlopin's  monograph  published  in  Russian 
and  entitled  "Coal  Tar  Dyes.  Classification,  properties,  and  action 
of  artificial  dyes  on  the  animal  organism,  etc.,"  published  at  Dorpat 
in  1903,  or  to  the  abstract  of  Chlopin's  paper  printed  at  page  169-172 
of  Vol.  IV  of  the  Report  of  the  Fifth  International  Congress  of  Ap- 
plied Chemistry  held  in  Berlin,  1903. 

"Canton  of  Tessin"  refers  to  the  publications  of  the  Tessin  regula- 
tions published  in  1897  in  Zeitschrift  fur  Untersuchung  dor  Nahrungs 
und  Genussmittel,  page  414. 

Whenever  possible  the  doses  administered  have  been  given  in  mil- 
ligrams per  kilo  and  grains  per  100  pounds  of  body  weight  of  animal. 
In  the  case  of  the  tabulations  taken  from  Chlopin's  monograph  this 
was  not  done;  but  in  order  to  render  such  comparative  data  easily 
available  factors  have  been  placed  at  the  head  of  each  tabulation; 
for  example,  under  G.  T.  6  (1  gram  =106  mg  =  74.2  grains),  which 
means  that  each  gram  administered  amounts  to  106  mg  per  kilo  or 
74.2  grains  per  100  pounds  of  body  weight  of  animal;  by  multiplying 
the  doses  given  by  either  of  the  factors  the  corresponding  compara- 
tive information  is  obtained. 

In  addition  to  the  106  Green  Table  numbers  that  have  been 
examined  physiologically,  there  are  reported  the  results  of  the  phys- 
iological examination  of  8  coal-tar  colors  mot  in  the  Green  Tables,  of 
which  3  are  said  to  be  nonpoisonous,  .'5  are  called  poisonous,  1  is 
called  harmful,  and  the  last  is  said  to  be  "nol  quite  harmless.' J 
These  8  dyes  are  qoI  included  in  this  compilation. 

TABULATION     Bl     GREEN     TABLE     NUMBERS    <>!      PHTSIOLOGICA]       \.\i> 

01  mi:    D  \  i  \. 

G.  T.  1. 

Tradi  mums. — Picric  acid;  carbazotic  acid. 
Scientific  narru  .—Symmetrical  trinitrophenol. 
Discovered. — 1771. 
Shade, — Yellow.     Not  offered. 


76  COAL-TAR   COLORS  USED  IN    FOOD  PRODUCTS. 

FAVORABLE. 

Nothing. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

2.  Weyl  (p.  30):  "The  injurious  character  of  picric  acid  has  long  been  known." 

3.  "In  Germany  its  employment  for  coloring  food  is  forbidden  by  the  imperial  enact- 

ment of  1888,  on  account  of  its  poisonous  character."     (pp.  68-71.) 

4.  "The  foregoing  statements  show  that  while  the  acid  must  be  considered  poisonous, 

its  injurious  character  is  far  less  than  has  generally  been  assumed,  nevertheless, 
the  legal  prohibition  of  its  use  as  a  coloring  matter  for  food  or  drink  is  just." 
(p.  71.) 

5.  "Erb  gave  a  rabbit  weighing  1,700  grams,  0.06  gram  of  potassium  picrate  (24.5 

grains  per  100  pounds)  daily  for  90  days;  slight  loss  of  weight  and  occasional 
diarrhea  were  noted,  but  nothing  more  serious."     (p.  69.) 

6.  A  rabbit  weighing  2,065  grams  died  at  the  end  of  19  days,  after  having  taken  2.52 

grams  of  the  substance,  or  854  grains  per  100  pounds  body  weight;  number  of 
doses  not  stated,     (p.  69.) 

7.  Weyl's  experiment  on  a  dog,  weight  not  given:  April  21-26,  0.24  gram  (3.7  grains) 

sodium  picrate  daily;  April  28-May  9,  0.36  gram  (5.5  grains)  daily;  total,  5.76 
grams  (8.9  grains)  sodium  picrate;  no  serious  disturbance;  May  13,  1.2  grams 
(18h  grains)  sodium  picrate  at  one  dose;  weakness  marked,  diarrhea  and  dyspnea 
next  day;  May  14,  0.6  gram  (9^  grains)  caused  vomiting;  evening  of  same  day, 
0.36  gram  (5.6  grains)  given;  May  15,  animal  lively;  0.24  gram  (3.7  grains) 
again  given,  and  on  evening  of  same  day  0.72  gram  (11.2  grains);  May  16, 
marked  weakness  of  animal,  and  0.16  gram  (2.5  grains)  given,  causing  vomiting; 
May  17,  0.17  gram  (2.6  grains)  given;  May  18  and  19,  animal  definitely  recovered, 
and  aside  from  strong  yellow  tinge  of  the  conjunctiva  and  skin,  no  abnormal 
conditions  manifest.  Animal  died  May  20  after  receiving  1.32  grams  (20.4 
grains)  potassium  picrate.  Weyl  concludes,  therefore,  that  dogs  are  resistant 
to  this  substance,  notwithstanding  the  prostration  and  the  blood  disorganiza- 
tion. 

8.  Weyl  summarizes  the  effect  on  humans  from  therapeutic  and  poisoning  cases  to 

the  effect  that  daily  doses  of  from  0.54  to  0.90  gram  (8.3  to  13.8  grains)  of  potas- 
sium picrate  are  easily  borne  by  healthy  adults  for  a  considerable  time;  children 
and  weak  adults  bear  picric  acid  badly,     (p.  70.) 

9.  "Picric  acid     *    *    *     is  poisonous    *    *     *."     (p.  96.) 

10.  Fraenkel  (p.  572):  "On  the  other  hand,  this  substance  is  not  usable  for  interna] 
administration  on  account  of  its  decomposing  the  red  blood  corpuscles,  and  of 
it  energetic  cramp  production,  as  well  as  on  account  of  its  disturbance  of  the 
kidneys,  and  the  ultimate  paralysis  of  the  respiratory  centers;  nevertheless, 
picric  acid  is  not  to  be  considered  a  violent  poison    *    *    *." 

11  Schacherl  (p.  1044):  "Picric  acid  *  *  *  (is),  according  to  numerous  state- 
ments in  the  literature,  poisonous  even  in  small  doses,  and  (is)  therefore  un- 
qualifiedly to  be  declared  as  impermissible." 

L2.  LlBBEB  (p.  16),  where  it  is  stated  to  be  forbidden  by  the  German  law,  aiul  is  also 
otherwise  substantially  the  same  as  Weyl  above  quote  I. 

i.;  Resolutions  "i"  tin-  Society  of  Swiss  Analytical  Chemists,  September,  L891:  "The 
following  are  to  be  regarded  a-  <  < » 1  < . r  i 1 1 lt  matters  harmful  to  health:  *  *  * 
picric  add    *    *    *." 

n.  Prohibited  by  the  Belgian  law  of  June  17,  L891. 

ii  l.i .win  (Lekrbuch der  Toxtkologiet  t897%  p.  lSt)\  "Picric  acid  is  poisonous.  Rab- 
bits Can  stand  daily  I"  milligrams  of  a  green  containing  picric  acid,  but  n<>(  L'O 

milligrams.    Their  death  Is  accompanied  by  paralysis." 

It;.    JJissli.-l     ii  ,i  ■  poisonous. 


COMPILED   DATA    UNDER   GREEN    TABLE    NUMBERS.  77 

G.  T.  2. 

Trade  names. — Victoria  Yellow;  Victoria  Orange;  Golden  Yellow; 
Saffron  Substitute;  Anilin  Orange;  Di-nitro-Cresol. 
Scientific  name. — Di-nitro-o-and-p-cresol. 
Shade. — Yellow.     Xot  offered. 
Discovered. — 1869. 
Used  for  coloring  butter,  liqueurs,  etc. 

FAVORABLE. 

Nothing. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

2.  Fraenkel  (p.  572):  "On  the  other  hand  dinitro-cresol  is  much  more  intensely 

poisonous  (than  picric  acid),  which  is  probably  caused  by  its  greater  solubility 
in  water." 

3.  Schacherl  (p.  1044):  *    *    *    Dinitro-cresol  [is],  according  to  numerous  state- 

ments in  the  literature,  poisonous  even  in  small  doses,  and  [is]  therefore  unquali- 
fiedly to  be  declared  as  unpermissible." 

4.  Resolutions  of  the  Society  of  Swiss  Analytical  Chemists,  September,  1891:  "The 

following  are  to  be  regarded  as  coloring  matters  harmful  to  health    *    *    * 
Dinitro-cresol    *    *    *." 

5.  Forbidden  by  the  Canton  of  Tessin. 

6.  Weyl  (p.  31):  "I  have  shown  the  same  (poisonous  nature)  for  Dinitro-cresol  (Saf- 

fron Substitute).     (See  Zts.  angew.  Chem.,  1888,  No.  12,  for  confirmation  of  my 
results  by  Gerlach.)" 

7.  "The  reverse  is  the  case  with  the  poisonous  dinitro-cresol  (Saffron  Substitute). " 

(P-  55.) 

8.  Weyl  describes  experiments  with  this  compound,     {pp.  71-85.) 

9.  Fourteen  rabbits  were  experimented  on,  of  which  13  died.     Amounts  administered 

in  the  fatal  cases  per  100  pounds  body  weight  were  {p.  74): 
Grains.  Grains. 

189  175 

175  168 

175  175 

175  168 

175  168 

175  175 

175 
Of  12  experiments  on  dogs,  5  receiving  the  color  by  the  mouth  and  7  hypoder- 
mically,  3  cases  resulted  fatally;  the  fatal  case  by  the  mouth  requiring  ;>s'.  grains 

1  >cr  LOO  pounds  body  freight ;  the  2  fatal  cases  hypodermically  represented  1 1  and 
20 grains  per  LOO  pounds  body  weight .  reaped  ively,  although  L40,  88.5,  :;i  .6,  and 

•-..in-  per  i<><>  pounds  body  weight  by  the  moutb  were  borne  without  fatal 
effect;  ami  lm^,  m  ad  4.9  grains  per  loo  pounds  body  weight,  hypo- 

dermically, wen-  also  borne  \\  ithout  fatal  effect  {p.  75). 
lo.  \Vi.yi.i'/>.  9€)'.    "*    *    *    Dinitro-cresol    *    *    *    are  [is] poisonous;    *    *    *" 
ii.  Prohibited  by  the  Belgian  law  of  June  it,  L801. 

Ztt.  Nahr.G  Eti   ommended  as  an  Insecticide,  L500  being 

sufficient  far  all  ordinary  purposes.    One  milligram  is  sufficient  to  kill  a  mouse; 

2  milligrams  recommended  f'>r  killim:  mice. 

]:;.  W'kvi.  ( HandbuA  der  Hygieru  i:  For  humans,  thefataldose,  when  administered  by 
the  stomach,  appears  t<>  be  no  milligrams  per  kil<>  body  weight,  or  48  graii 
100  pounds. 


78  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

14.  "The  president  of  the  Council  of  Oppeln  forbids  on  April  19,  1899,  the  use  of  Saf- 

fron Surrogate  for  coloring  food  products." 

15.  Lewint  (Lehrbuch  der    Toxikologie,   1897,  p.  232):   "Saffron   Surrogate    *    *    *, 

which  is  used  for  coloring  foodstuffs,  is  poisonous.  It  appears  to  attack  the 
coloring  matter  of  the  blood,  and  produces,  in  the  case  of  dogs,  vomiting,  cramps, 
and  convulsions.  *  *  *  Feathers  colored  with  Saffron  Surrogate  cause 
burning  and  itching,  and  finally  blisters  on  the  hands  of  the  women  working 
with  them;  the  faces  were  also  similarly  affected,  and  this  was  accompanied  by 
loss  of  appetite  and  fever." 

16.  Buss  lists  it  as  poisonous. 

G.  T.  3. 

Trade  names. — Martius  Yellow;  Naphthol  Yellow;  Naphthylene  Yel- 
low; Naphthylamin  Yellow;  Manchester  Yellow;  Golden  Yellow;  Saf- 
fron Yellow;  Jaune  d'Or;  Jaune  Naphthol. 

Scientific  name. — Dinitro-alpha-naphthol. 

Discovered. — 1864. 

Shade. — Yellow.     Not  offered. 

FAVORABLE. 

Nothing. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

2.  Weyl  (p.  31):  "Cazeneuve  and   Lepine  pointed  out  the  poisonous  nature  of 

Martius  Yellow    *    *    *." 

3.  "This  body  (Chamber  of  Commerce  at  Sonneberg)  recommends  for  the  prepara- 

tion of  children's  toys  three  colors,  the  poisonous  character  of  which  I  can 
demonstrate.     These  are  Martius  Yellow    *    *    *."     (p.  34.) 

4.  "For  instance,  for  preliminary  researches,   dogs  and  rabbits  have  value   for 

chemical  reasons.  The  conclusions  derived  from  such  experiments  must  be 
accepted  with  great  deliberation,  since  it  happens  that  rabbits  will  bear  without 
injury  doses  which  will  seriously,  nay,  even  fatally,  act  upon  the  dog,  as  I 
have  already  shown  to  be  the  case  with  Martius  Yellow."     (p.  56.) 

5.  Where  two  experiments  by  Cazeneuve  and  Lepine  are  referred  to,  in  which 

diarrhea,  vomiting,  and  albuminuria  were  produced  by  this  substance. 
(pp.  85-89.) 

6.  Weyl's  own  experiments  on  4  dogs  showed  weakness,  vomiting,  diarrhea,  and 

albuminuria  resulting  from  the  use  of  this  color;  the  amounts  of  color  admin- 
istered per  kilogram  of  body  weight  were  73,  17.5,  17.5,  and  11.3  milligrams, 
which  amount  to  51,  12,  12,  and  8  grains,  respectively,  per  100  pounds  of 
body  weight,     (p.  87.) 

7.  "Martius  Yellow,  therefore,  belongs  to  the  injurious  colors.     As  a  coloring  matter 

for  food  and  drink  its  use  should  be  wholly  prohibited."     (p.  89.) 

8.  "*    *    *    and  Martius  Yellow  are  poisonous;    *    *    *."     (p.  96.) 

'i  l.cwiv  ( Lehrbuch  der  Toxikologie,  t897t  j>.  tSl):  "Like  Saffron  Surrogate,  it  is 
poisonous.  In  an  experiment  on  myself,  using  large  doses,  I  noticed  among 
others  Ihe  general  yellow  coloration  of  the  skin.  In  a  poisoning  resulting 
fatally  after  5  hours  with  Martins  Yellow,  vomiting,  yellow  coloration  of  the 
skin  and  mucous  membranes  were  observed;  whereas  the  autopsy  revealed, 
among  other  things,  hemorrhagic  gastritis,    (Jacobson,  Hosp.  Tid.,  18W,  p. 


COMPILED  DATA   UNDER   GREEN    TABLE    NUMBERS.  79 

10.  "  Such  small  amounts  as  are  used  for  the  coloring  of  pastry  are  said  to  be  non- 

poisonous.     ( Vitalil  boll,  chim.farm.,  1893,  p.  738.)"     (p.  231.) 

11.  Cazeneuve  and  Lepine  (Compt.  rend.,  1885,  v.  101,  pp.  1167-1169)  say:  I.  "A 

dog  received  71  milligrams  per  kilogram  of  body  weight,  or  50  grains  per  100 
pounds  daily.  On  the  second  day  diarrhea  and  vomiting  ensued;  loss  of 
appetite  except  for  milk.  Thereafter  it  experienced  difficulties  in  breathing; 
suffered  albuminuria;  its  urine  was  colored;  it  died  on  the  sixth  day.  The 
autopsy  disclosed  considerable  congestion.  II.  A  dog  weighing  22  kilo- 
received  400  milligrams  (19  milligrams  per  kilo  or  13  grains  per  100  pounds); 
this  caused  a  yellow  vomit;  next  day  it  received  500  milligrams  (27  milligrams 
per  kilo  or  17  grains  per  100  pounds),  which  caused  violent  diarrhea,  fever, 
thirst,  disinclination  for  all  food.  The  animal  was  killed;  the  autopsy  showed 
badly  congested  kidneys." 

12.  Prohibited  by  the  Belgian  law  of  June  17,  1891. 

13.  Schacherl  (p.  1044)'-     "*    *    *    Martius  Yellow    *    *    *    [is],  according    to 

numerous  statements  in  the  literature,  poisonous  even  in  small  doses,  and  [is] 
therefore  unqualifiedly  to  be  declared  as  unpermissible." 

14.  Prohibited  by  law  in  Italy.     (See  Lieber,  p.  24.) 

15.  Fraenkel  (p.  572):  "This  substance  also  shows  poisonous  properties,  although 

it  is  less  poisonous  than  dinitro-cresol." 
10.  Resolutions  of  the  Society  of  Suiss  Analytical  Chemists,  September,   1891:  "  The 
following  are  to  be  regarded  as  coloring  matters  harmful  to  health     *    *    * 
Martius  Yellow    *    *    *." 

17.  Forbidden  by  the  Canton  of  Tessin. 

18.  Dietrich  (Zts.  Nahr.  Genussm.,  1902,  v.  5,  p.  364)'-  "A  lot  of  groats,  after  eating 

which  a  family  became  sick,  was  found  to  be  free  from  ordinary  poisons,  but 
had  been  colored  with  Martius  Yellow." 

19.  Buss  lists  it  as  poisonous. 

DOUBTFUL. 

1.  Winogradow  (Zts.  Nahrs.  Genussm.,  1903,  v.  6,  p.  589)  says  it  noticeably  retards 
digestive  action;  is  not  indifferent. 

G.  T.  4. 

Trade  names. — Sulphur  Yellow;  Sulphonaphthol  Acid  Yellow: 
Succinic;  Solid  Yellow;  Saffron  Yellow:  Jaune  Acide  (\:  Jaune  Acide; 
Fasl   Yellow;  Citronin;  Anilin  Yellow  ;  Acid  Yellow  S. 

Names  und<  r  which  it  was  offered  on  'tin    United  States  market  as  <i 

food  color  in  1907.-  NTaphthol   Yellow  SLOZ;   Naphthol   Yellow  S; 

Naphthol  Yellow:  Naphthol  Yellow  L;  Yellow  I-'  V:  Lemon  Yellow. 

Scit  nti/ic  nana .      Dinil  i <     ilplii-naphthol-beta-monosulphonic  acid. 

Discovered  and  i»it<  nt<</.     1879, 

Shade.     V<'ll«>w.     Offered  by  10  out  of  L2  soun 

I  A\  <>l;  Alii  | 

I.  Permitted  by  ( kmfecl Loners'  !.i.-t . 

\/i\m\i    wi.  I  mim    {Compt  rend.,  Wl,  pp.  1167-1169):  ■  A  dog 

day  for  5  days  32  milligrams  per  kilogram  of  body  weight,  «>r 

2:\  grains  per  n><>  pounds;  for  the  i<>  days  next  rfu<    i  ived  four  times 

that  amount,  that  i-.  L33  milligrams  per  kilogram  ol  body  \\<'i'.:lit.  or  93  grains 


80  COAL-TAR   COLORS   USED   IX   FOOD  PRODUCTS. 

2.  Cazeneuve  and  Lepine  (Compt.  rend.,  1885,  v.  101,  pp.  1167-1169) — Continued. 

per  100  pounds;  for  the  10  days  next  succeeding  it  received  daily  twice  the  last 
amount,  or  266  milligrams  per  kilogram  of  body  weight,  that  is,  186  grains  per 
100  pounds.  It  received  altogether  in  the  25  days  62£  grams,  or  964  grains. 
There  was  no  vomiting,  no  diarrhea,  and  no  albumen  in  the  urine  at  any 
time." 

3.  Weyl  (p.  31):  "*    *    *    not  poisonous  to  human  beings  and  dogs:  Naphthol 

YellowS.     *    *    *." 

Weyl  describes  his  own  experiments  on  3  dogs,  giving  them,  respectively, 
417,  34,  and  100  milligrams  per  kilo  body  weight,  or  per  100  pounds  292,  24, 
and  70  grains,  respectively.  Whether  the  color  was  administered  by  the  mouth, 
or  injected  subcutaneously,  all  bodily  functions  appeared  to  remain  normal, 
and  it  was  only  in  the  case  of  repeated  doses  of  417  milligrams  per  kilogram 
of  body  weight,  or  292  grains  per  100  pounds,  that  albuminuria  appeared. 
{pp.  89-92.) 

4.  "Only  the  sulphonated  colors  Naphthol  Yellow    *    *    *    are  harmless  and  appli- 

cable to  the  coloring  of  food  and  drink."     (p.  96.) 

5.  Permitted  by  the  laws  of  Austria. 

6.  Permitted  by  the  law  of  Italy. 

7.  Permitted  by  the  law  of  France. 

8.  Schacherl  (p.  1044)'  "*    *    *    Naphthol  Yellow  S    *    *    *    possesses  no  poi- 

sonous properties." 

9.  Fraenkel  (p.  572):  "Naphthol  Yellow  S  is  an  entirely  nonpoisonous  substance." 

10.  Meyer  (/.  Amer.  Chem.  Soc.  1907,  v.  29,  p.  900):  One  hundred  milligrams  per 

kilogram  of  body  weight  for  the  initial  administration,  and  subsequent  admin- 
istrations increased  geometrically.  After  the  second  administration  intermit- 
tent diarrhea  resulted,  emphasized  by  increased  amounts  with  no  albumin  or 
sugar  in  the  urine;  continued  for  14  administrations;  60  that  in  14  administra- 
tions 147.58  grams  of  color  had  been  given;  the  initial  dose  is  70  grains  per  100 
pounds  of  body  weight,  and  the  average  daily  dose  of  the  total  administered 
is  394  grains  per  100  pounds  of  body  weight.  Urine  only  slightly  yellow  col- 
ored after  small  doses,  but  red  after  larger  doses. 

11.  Lieber  (p.  14S):  A  dog  received  36  milligrams  per  kilogram  of  body  weight,  or 

25.2  grains  per  100  pounds  once  a  day  seven  times  every  other  day;  during  the 
whole  period  the  dog  was  apparently  in  good  condition  with  no  bad  effects 
from  the  color. 

12.  Buss  lists  it  as  nonpoisonous. 

13.  Cazeneuve   and   Lepine  (Compt.  rend.,    1885,    v.   101,  pp.   1167-1169):  Three 

chronic  invalids  received  daily  from  2  to  4  grams  of  the  dye  in  cocheta;  except 
slight  colic  and  diarrhea  nothing  abnormal. 

DOUBTFUL. 

1.  Lewin  (Lehrbuch  der  Toxikologie,  1897,  p.  282):  "Acid  Yellow  S  is  said  to  be  able 

t'»  produce  <  1«tiiki j it i ~  -Hi  frequent  contact  therewith." 

2.  WlNOORADOW  {Zls.  Nulir.  Qenuum.,  1908,  v.  6,  p.  589)  says  it  noticeably  retards 

digestive  action;  ianol  indifferent. 

G.  T.  5. 

Trade  name. — Brilliant  Yellow;   Naphthol  Yellow  S  or  RS. 
Scientificnantc. — Dinit  m-alplia-naphthol-alpha-monosulphonicacid. 
Discovered  and  patented. — 1884. 
Shade. — Yellow.     Not  offered. 


COMPILED   DATA   UNDER    GREEN    TABLE    NUMBERS. 


81 


FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (pp.  92-94)'-  Describes  experiments  on  2  dogs,  in  which  the  initial  dose 

was  532  milligrams  by  the  mouth,  and  17  milligrams  hypodermieally,  per  kilo- 
gram of  body  weight,  respectively,  372  and  12  grains  per  100  pounds  of  body 
weight;  in  both  cases  the  urine  was  colored,  in  the  second  case  traces  of  albu- 
minuria resulted.     In  the  first  case  the  albuminuria  was  doubtful. 

3.  "Brilliant  Yellow  is  not  poisonous,  even  in  large  doses,  when  administered  by  the 

stomach     *     *     *     the  albuminuria  was  very  slight,     (p.  94-) 

4.  "Only   the   sulphonated   colors    *    *    *     Brilliant  Yellow,   are   harmless,    and 

applicable  to  the  coloring  of  food  and  drink.  "     (p.  96.) 

5.  Schacherl     (p.     1044)'-  "     *     *     *     Brilliant     Yellow     *     *     *     possesses    no 

poisonous  properties. " 

6.  Fraenkel  (p.  572):  "For  the  same  reason     * 

is  without  effect. " 

G.  T.  6. 


*    Brilliant  Yellow 


Tradenames. — Aurantia;    Nitrodiphenylamin;    Imperial    Yellow 
Kaiser  Yellow. 

Scientific  name. — Hexanitro-diphenylaniin. 

Discovered. — 1873. 

Shade. — Yellow.     Not  offered. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


*  Aurantia  suspicious.  " 

*  *    *    Aurantia  [is]  according  to  numerous  statements 


1.  Weyl  (p.  00):  "    * 

2.  Schacherl  (p.  1044) 

in  the  literature  poisonous  even  in  small  doses,  and  [is]  therefore  unqualifiedly 
to  be  declared  as  impermissible.  " 

3.  Chlopin  {p.  1 16)  as  results  of  his  experiments  considere  it  injurious.    The  experi- 

mental <lata  are  as  follows: 

Omental  data  by  Chlopin. 

[1  Kram  =  10G  mg«=74.2  grains.] 


lm  boon' 
urine. 

<  inn-nil  condition  Of  animal  ami  urine. 

Mar.    12 

i 

2 
3 

3 

:< 

re. 
MO 

uo 
no 

:  Intent  urine  an<l  dog  normal 

14 

l  vomiting;  urine  dark                   1;  do  albumen;  dog 
omiting;  urine  aim                    Id;  no  albumen 

U 

Is 

L0 

a 

n 

Same;  urine  i 

lion  normal. 
Qradually  color  Of  Ul                      M  normal;  in  c\.t\  ofbei 

\Ncll. 

Lfl 

97291       r.wll    I  i.     [2 G 


82  COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

4.  Fraenkel  (p.  573):  "The  coloring  matter  called  Aurantia,  which  is  a  salt  of 

hexanitro-diphenylamin,  appears  to  be  poisonous  on  account  of  the  nitro  groups, 
which  is  on  the  other  hand  denied  by  a  few  observers. " 

5.  Resolutions  of  the  Swiss  Analytical  Chemists,  September,  1891:  "The  following  are 

to   be   regarded   as   coloring   matters  harmful   to  health    *    *    *    Aurantia 


r>.  Forbidden  by  the  Canton  of  Tessin. 

7.  Lbwin  (Lehrbuch  der  Toxihologie,  1897,  p.  232):  "Aurantia  has  a  poisonous  action. 

Alter  wearing  gloves  for  8  hours  made  with  so-called  dogskin,  which  were  col- 
ored with  Aurantia,  a  man  suffered  confluent  blisters,  accompanied  by  itching. 
The  workmen  with  this  material  get  blisters  on  the  face  and  on  the  hands. 
Perspiration  increases  the  tendency  to  such  blisters." 

8.  Buss  lists  it  as  poisonous. 

G.  T.  8. 

Trade  names. — Acid  Yellow;  Fast  Yellow  G;  Acid  Yellow  G;  Fast 
Yellow;  Fast  Yellow  extra;  Jaime  Acide;  New  Yellow  L. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907.— Fast  Yellow  Y;  Fast  Yellow  G;  Acid  Yellow  G 
pat.;  Fast  Yellow  053. 

Scientific  name. — Amidoazobenzene-disulphonate  with  some  sodium 
amidoazobenzene-monosulphonate. 

Discovered. — 1878. 

Shade. — Yellow.     Offered  by  5  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Cazeneuve  and  Lepine  (Bull,  de  Vacad.  de  med.,  April  27,  1886,  p.  643),  where 

it  is  classified  among  the  "nontoxic  "  colors. 
:;.  Fraenkel  (p.  575),  where  it  is  stated  to  be  nonpoisonous. 
4.  Permitted  by  the  law  of  Austria. 

UNFAVORABLE. 

1 .  Weyl  (p.  115):  "Poisonous  to  human  beings.     (?)" 

2.  Chlopin  (p.  151)  considers  that  the  work  of  others  makes  this  a  suspicious  color. 

1 1  is  own  experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 

<;.  T.  8  AND  9. 

[i  grain  -152  mg— 106  grains.] 


Weight. 

24  hours' 
urine. 

( fenei  \i  oondltton  of  animal  and  mine. 

1901. 

LI   13 

Grams. 

Kih.s. 

cc. 
310 

Dog  normal;  color  urine  normal;  add;  no  albumen. 

it 

1 

6.6 

Do. 

IS 

Do, 

Lfl 

Urine  greenish  brown;  reddens  with  HsSO<  and  HQ;  no 

17 

880 
820 

albumen. 
Color  same;  traoea  of  albumen 

Is 

Color  leas  Intense;  trace  of  albumen. 

I'.t 

Do. 
Urine  greenish  brown;  albumen  gone;  dog  is  lively. 

21 

202 

Everything  normal. 

Total 

4 

(  oncluaion;  "Suspicious," 


COMPILED  DATA  UNDER  GREEN   TABLE    NUMBERS.  83 

3.  Buss  (Forschungsber.  iiber  Lebensmittel,  1896,    Vol.  Ill,  p.  173):  Is  regarded  as 

poisonous. 

4.  Robert  (Lehrbuch  der  Intoxicationen,  1893,  p.  335):  Listed  as  poisonous. 

5.  Lewin  (Lehrbuch  der  Toxikologie,  1897,  p.  231)  says  "produces  eczema,"  and 

cites  Deutsche  Med.  Wochenschr.,  1891,  p.  45. 

G.  T.  9. 

Trade  names. — Fast  Yellow  R;  Fast  Yellow;  Yellow  W. 
Name  under  which  it  was  offered  on  the   United  States  market  as  a 
food  color  in  1907.— Fast  Yellow  034. 

Scientific  name. — Sodium  salt  of  amidoazotoluene-disulphonic  acid. 

Discovered  and  patented. — 1878. 

Shade. — Yellow.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  31):  u     *    *    *    not  poisonous  to  human  beings  and  dogs    *    *    * 

Solid  Yellow." 

3.  Cazeneuve  and  Lepine  (Compt.  rend.,  1885,  v.  101,  pp.  1167-1169):  A.  A  dog 

received  42  milligrams  per  kilogram  of  body  weight,  or  29  grains  per  100  pounds, 
for  5  days;  thereupon  received  four  times  that  amount  for  5  days,  or  168  milli- 
grams per  kilogram  body  weight,  or  117  grains  per  100  pounds;  for  the  10  days 
next  succeeding  it  received  daily  twice  the  last  dose,  or  336  milligrams  per 
kilogram  of  body  weight,  that  is,  235  grains  per  100  pounds;  it  then  received 
in  1  day  20  times  the  original  dose,  or  840  milligrams  per  kilogram  body 
weight,  that  is,  596  grains  per  100  pounds,  and  during  the  entire  period  nothing 
abnormal  was  noticed.  B.  Three  chronic  invalids  received  from  2  to  4  grains 
of  the  dye  daily;  except  colic  without  diarrhea  nothing  abnormal.  They  con- 
cluded that  this  dye  is  no  more  harmful  than  Naphthol  Yellow  S  (G.  T.  I  . 

4.  Cazeneuve  and  Lepine  (Bull,  de  Vacad.  dc  mcd.,  1886,  p.  643):  Tolerated  by 

man,  well  or  sick. 

I    \ FAVORABLE. 

1.  Weyl  (p.  115):  "Poisonous  to  human  beings.     (?)" 

2.  Chlopin  (p.  151):  Where  he  considers  that  the  work  of  others  makes  this  a  sus- 

picious color.    For  his  experimental  data  thereon  sec  table  under  G.  T.  8; 
Chlopin's  chemical  description  of  the  dye  used  applies  to  both  Q.  T.  8  and  9. 
:;.  Cobibt   Lekrbv/ch  der  Intoxicationen,  t893,p.SS€):  Listed  as  poisonous. 

G.  T.  11. 

Tradi  names. — Sudan  I ;  Carminaph. 

Na/ms  a  a  J, /•  which  it  was  offered  on  Qu    United  States  market  as  a 
food  <<>h>r  in  1907.  —oil  Orange  7078j  Geraaio  Orange  I. 
Scientific  name. — Benzene-azo-betanaphthol. 

Pi  scon  mi.      L883. 

Shade,     Orange  Yellow.     Offered  by  2  out  of  11*  sources. 

i  LVOB  mii  I. 

1.  Wan  "Nonpoisonous    *    *    *    Soudan  I    *    *    *." 

2.  "  Other  Aso-colors,    *    *    *    for  instance  Soudan  I     •     *    ■    are  entirely  non- 

poisonous,"    '/>.  / 


84  COAL-TAR   COLORS  USED  IN   FOOD  PRODUCTS. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

2.  Weyl  (p.  119):  Dog  received  18  grams  in  6  doses  in  17  days,  and  remained  under 

observation  5  days  longer;  4  doses  of  168  milligrams  per  kilogram  body  weight 
(118  grains  per  100  pounds)  and  2  doses  of  420  milligrams  per  kilogram  body 
weight  (294  grains  per  100  pounds)  produced  colored  urine,  phenol  in  urine, 
vomiting  and  distinct  albuminuria  beginning  with  the  third  dose.  From  the 
foregoing  Weyl  concludes  as  follows:  "The  color  in  the  doses  administered  is 
not  entirely  harmless,  since  a  limited  albuminuria  seems  to  be  brought  about." 

3.  Fraexkel  (p.  576):  u  It  is  not  wholly  harmless,  since  this  coloring  matter  seems 

to  produce  a  slight  albuminuria.'1 

G.  T.  13. 

Trade  names. — Ponceau  4  GB;  Crocein  Orange;  Brilliant  Orange; 
Orange  GEX. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Crocein  Orange  10234;  Crocein  Orange;  Crocein 
Orange  G;  Ponceau  4  GB. 

Scientific   name. — Anilin-azo-betanaphthol-monosulphonic   acid. 

Discovered. — 1878. 

Shade. — Orange  Yellow.     Offered  by  6  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  115):  "Nonpoisonous    *    *    *    Ponceau  4  G  B    *    *    *.*' 

3.  Experiment  on  dog  in  doses  of  161  milligrams  per  kilogram  body  weight;  that  is, 

113  grains  per  100  pounds  body  weight,  apparently  produced  no  disturbance 
aside  from  coloring  of  the  urine,     (p.  124.) 

4.  Weyl  (p.  148):  "Other  Azo-colors    *    *    *    for  instance    *    *    *    New  Coc- 

cin    *    *    *    are  entirely  nonpoisonous. " 

5.  Weyl's  conclusion  reads  as  follows:  "This  color  can  be  regarded  as  nonpoisonous." 

6.  Fraexkel  (p.  577):  "Ponceau  4GB  can  be  regarded  as  nonpoisonous." 

UNFAVORABLE. 

1.  Excluded  by  law  of  Ac  stria. 

G.  T.  14. 

Trade  names. — Orange  G;  Orange  G  G. 

Names  under  which  it  was  offered  on  the  United  Stat<s  market  as  a 
food  color  in  1007. — Orange  G  G  crystals;  Orange  G. 
Scientific  name.  -Anilin-azo-betanaphthol-disulphonic  acid  G. 
Di8covi  r<  d  and  pato  nted. — 1878. 
Shade. — Orange  Yellow.     Offered  by  2  out  of  12  sources. 


COMPILED  DATA  UNDER  GREEN   TABLE   NUMBERS. 


85 


FAVORABLE. 

1.  Chlopin  examined  this  color,  and  his  experimental  data  are  as  follows: 
Experimental  data  by  Chlopin. 
No.  1  (p.  12S). 
[1  gram=73  mg=51  grains.] 


Date. 

Dose. 

Weight. 

24-hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Apr.    4 

Grams. 

1 

Kilos. 
13.7 

cc. 
525 
600 
990 
550 
680 
730 
755 

Nothing  abnormal;  no  albumen. 

Urine  light  chocolate  brown,  acid;  no  albumen. 

6 

2 

Urine  clear,  yellow,  blackish  sheen;  no  albumen. 

7 

Urine  clear,  dark  brown;  no  albumen;  faintly  alkaline. 

8 

Do. 

9 

Nothing  abnormal. 

10 

Do. 

Total. 

3 

No.  2  (p.  124). 
[1  gram=119  mg=103  grains.] 


1901. 
Nov.    8 

8.4 

315 

12 

3 

13-14 

370 

15 

3 
3 
3 

3 

16 

250 
320 
210 
225 
295 

17 

18 

20 

21 

Total  . 

15 

Nothing  abnormal;  no  albumen. 

Do. 
Urine  orange  in  color,  acid,  no  albumen;  in  other  respects  nothing 
abnormal. 

Do. 

Do. 

Do. 

Do. 

Do. 

Do. 


Conclusion:  Nonpoisonous. 


1.  Excluded  by  Austrian  law. 


UNFAVORABLE. 


G.  T.  15. 


Trade  names. — Ponceau  2  G;  Orange  R. 

Scientific  name. — Sodium  salt  of  benzene-azo-beta-naphtlml-disul- 
phonic  acid  R. 
Shade. — Bright  Red.     Not  offered. 


FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

I    \1  AVOHAIII.K. 


1.  Kxrluded  under  Austrian  law 

2.  Excluded  under  Bwia  lawi 


G.  T.  16, 


TracU  names.     Butter  fellow;  Oil  Yellow. 

Scii  litific  uaim  .      Dinicthvl-uiiiido-u/o-lxMizcnc. 

Discovered.  -1875. 

Shade- -Yellow.     Not  offered. 


86 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


FAVORABLE. 

1.  Weyl  (p.  31):  "Butter  Yellow  produces  no  disturbance  in  rabbits." 

UNFAVORABLE. 

1.  Chlopin  (p.  138):  Where  as  a  result  of  his  own  experiments  he  considers  it  poi- 
sonous.    Ilis  experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 

No.  l. 

[1  gram=159  mg=lll  grains.] 


Date. 

Dose. 

Weight. 

General  condition  of  animal  and  urine. 

1902. 
May        6 

7-8 

Grams. 
3 

Kilos. 
6.3 

Before  experiment  urine  normal;  after  a  few  hours  vomiting;  urine  not 

collected. 
No  vomiting;  eats  poorlv;  more  tired  than  usual. 

9-15 

Dog  gradually  becomes  normal. 

16 



Vomiting;  loss  appetite. 

17 

Repeated  vomiting. 
Vomiting  continues.1 

18 



1 

No.  2. 
[1  gram=96  mg=67  grains.] 


1903. 
Feb.       5 


23 

10.4 

Before  experiment  dog  quite  normal;  acid;  no  albumen. 

Vomiting  during  night;  dog  does  not  eat,  but  drinks;  urine  more  yellow 

than  normal;  acid;  no  albumen;  in  the  evening  the  dog  waited  and 

drank  water. 
Died  during  the  night;  thin  excreta  in  kennel;  autopsy  showed  paralysis 

of  heart  as  causing  death. 


No.  3. 
[1  gram=167  mg=117  grains.] 


1903. 

Feb.       8 

9 

10 

11 

12 

13 
14-16 

17 
18 
19 


82  6 

32    



:>.  7 


Five  hours  after  administration  vomiting  and  involuntary  thin  feces. 
Dog  does  not  eat;  drinks  much;  weak;  urine  dark  yellow;  no  vomiting. 

Do. 
Dog  lies  in  cage;  moves  slowly  when  allowed  out  of  cage;  in  the  evening 

retching. 
Dog  is  still  weak,  but  general  condition  somewhat  better;  urine  strikingly 

colored;  acid;  no  albumen. 
Began  to  eat;  no  albumen. 
General  condition  improving  and  almost  normal;  lassitude  continues 

more  than  usual;  urme  normal  color;  acid;  do  albumen. 
In  the  evening  repeated  vomiting;  lossofapetite. 
No  vomiting;  in  the  evening  bothersome;  does  not  eat. 
Stools  normal;  striking  disturbance  of  movements;  paralysis  of  legs;  must 

spread  hind  legs  to  stand;  when  pushed  not  only  falls, "but  turns  on  his 

back;  sight  and  hearing  are  normal;  dog  died  at  night. 


1  I  his  dog  ran  away 


-  Qrueblor's  make. 


Berlin  make. 


G.  T.  17,  18,  41. 

17.    Trade  names. — Chrysoidin  Y;  Clirvsonliii  crystals. 
Name  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907,—  Ghrysoidiu  V. 

Scientific  name. — Anilin-azo-meta-phenylene-diamin. 
Discovered.  —1875. 


COMPILED   DATA    UNDER    GREEX    TABLE    NUMBERS.  87 

Shade. — Orange.     Offered  by  2  out  of  12  sources. 

18.  Trade  names. — Chrysoidin  R;  Cerotin  Orange;  C  extra;  Gold 
Orange  for  cotton. 

Name  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Chrysoidin  R. 

Scientific  name. — Anilin-azo-meta-tolylene-diamin. 

Shade. — Yellow  brown.     Offered  by  1  out  of  12  sources. 

41.   Trade  name. — Chrysoidin  R. 

Scientific  name. — Hydrochlorid  of  toluene-azo-meta-tolylene-di- 
amin. 

Discovered. — 1876. 

Shade. — Orange  Brown. 

(Note. — It  has  not  been  possible  accurately  to  differentiate  in  the  literature  as  to 
whether  Nos.  17,  18,  or  41,  or  all  three,  were  referred  to.) 

FAVORABLE. 

1.  V/eyl  (p.  115):  "  Nonpoisonous    *    *    *    Chrysoidin    *    *    *. " 

2.  Permitted  by  the  law  of  Italy. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

2.  Weyl  (p.  126):  Experiment  on  dog,  giving  him  113  milligrams  per  kilogram  body 

weight,  or  79  grains  per  100  pounds  body  weight,  produced  a  slight  albuminuria. 
In  a  second  experiment  a  dog  receiving  "1  grain"  ("grain"'  is  evidently  a 
misprint  for  "gram"  and  will  be  so  treated),  that  is,  105  milligrams  per  kilogram 
body  weight,  or  74  grains  per  100  pounds  body  weight,  daily  for  one  month,  did 
not  produce  albuminuria,  but  caused  a  lossof  body  weight  of  about  12.5 percent. 
A  third  dog  receiving  about  2  milligrams  per  kilogram  body  weight,  or  about  1.5 
grains  per  100  pounds  body  weight  subcutaneously,  suffered  a  loss  of  20  per  cent 
of  its  body  weight  in  23  days;  dose  repeated  24  days  after  and  animal  kept 
under  observation  seven  days  longer  when  animal  was  normal. 

3.  Weyl  in  summarizing  experiments  on  these  three  dogs  concludes  as  follows: 

"Chrysoidin  produces,  according  to  my  investigations,  a  slight  albuminuria, 
and  notable  reduction  in  body  weight,  but  further  disturbance  has  aol  been 
noted."     {p.  127.) 

4.  Fraexkel  (/).   577):  "The  abovo-iiKiitioned    Chrysoidin     *     *     *     produ 

slight  albuminuria,  and  a  notalAc  decrease  of  body  weight,  and  producet  factory 
eczema." 

5.  Lewin  (Lekrbuch  der  Toxikolo;  p.  IS1)\  "  Produces  eczema/'  and  cites 

Deutsche  Med.   Wnchatschr.,  1891,  p.  45. 

G.  T.  28. 
Trade  name. — Archil  Substitute  Y. 

Sen  ittific  naiitt  .  —  Sodium  salt  of  |>ara-nit  lolxMixeiie-a/o-alplia-na  j>h- 

bhylamin-para-sulphonic  add. 
Discovi  red  and  paU  nted.—l&7&. 

Shwl< . — Red.     Not  offered. 


88  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  \Veyl(p.  115):  "Nonpoisonous    *    *    *    Archil  Substitute     *    *    *." 

Describing  experiments  on  three  dog3,  as  follows:  A.  430  milligrams  per 
kilogram  body  weight,  or  301  grains  per  100  pounds  body  weight,  on  each  of  two 
successive  days,  and  double  the  dose  on  the  fourth  day,  producing  no  vomiting, 
but  a  tendency  to  vomit,  a  slight  albuminuria  and  colored  urine.  B.  182  mil- 
ligrams per  kilogram  body  weight,  or  L27  grains  per  100  pounds  body  weight, 
administered  daily  for  one  month;  results  similar  to  foregoing,  but  no  colored 
urine.  C.  105  milligrams  per  kilogram  body  weight ,  or  116  grains  per  100  pounds 
body  weight  administered  subcutaneously,  produced  only  slight  albuminuria, 
and  no  reduction  in  body  weight,     (p.  125.) 

G.  T.  43. 

Trade  names. — Orange  GT;  Orange  RN;  Orange  O;  Orange  N. 
Scientific  name. — Sodium  salt  of  toluene-azo-beta-naphthol-sulpho- 
nic  acid. 

Discovered. — 1879. 

Shade. — Orange.     Not  offered. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

UNFAVORABLE. 

1.  Excluded  by  Austrian  law. 

2.  Excluded  by  Swiss  laws. 

G.  T.  55. 

Trade  names. — Ponceau  R;  Ponceau  2  R;  Ponceau  G  and  GR; 
Xylidin  Red;  Xylidin  Scarlet. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Scarlet;  Orange  R. 

Scientific  name. — Sodium  salt  of  xylene-azo-bcta-naphthol-disul- 
phonic  acid. 

Shade. — Scarlet.     Offered  by  2  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioner-'  List. 

2.  Weyl  (p.  31):  "According  to  Cazeneuve  ami  Lepine'e  experiments  the  follow- 

ing are  not  poiaonous  to  human  beings  and  doge    *    *    *    Ponceau  R   *   *   *." 
'A.  "Ponceau  K  (Ponceau  2  R,  Xylidin  Red,  Xylidin  Ponceau),  not  poisonous  to  dogs 

neither  by  administration  by  stomach  n<>r  injection  into  blood."    (p.  115.) 
4.  "Other  Azo  colors    *    *    *    Xylidin  Red    *    *    *    are  entirely  nonpoisonous." 

{p.  lis.) 
:>.  Fbainxbl(p.575):  "Thatthe  monazo  coloring  matters  examined  by  Caseneuve 

mid  I /pi  n<\  as  already  above  stated,  were  nonpoisonous,  can  be  easily  explained 

by  the  constitution  <>f  these  substances.    These  two  investigators  examined 

*    *    *    Ponceau  It    *    *    *." 


COMPILED   DATA  UNDER   GREEN    TABLE    NUMBERS. 


89 


6.  Lieber  (p.  140):  A  guinea  pig  received  310  milligrams  per  kilogram  body  weight 

or  217  grains  per  100  pounds  body  weight,  once  a  day  six  times  ever}-  other  day; 
the  appetite  appeared  to  remain  good,  and  no  disturbances  were  noted. 

7.  Permitted  by  Austrian  law. 

8.  Permitted  by  Swiss  laws. 

9.  Cazexeuve  and  Lepixe  (Bull,  de  Vacad.  de  mid.,  1886,  p.  643):  Tolerated  by 

man  well  or  sick. 
10.  Chlopin  {p.  150)  classes  it  as  nonpoisonous  on  his  own  experiments.     His  experi- 
mental data  are  as  follows: 

Experimental  data  by  Chlopin. 
[1  gram=141  mg=  99  grains.] 


Date. 

Dose. 

Weight. 

24-hours' 
urine. 

General  condition  of  animal  and  urine. 

1902. 
May     3 

Grams. 
2 

Kilos. 
7.1 

cc. 
370 
351 
420 
290 
359 
360 
330 

Dog  and  urine  normal  and  no  albumen. 
Urine  rose-colored;  no  albumen. 

5 

2 

Color  normal;  no  albumen. 

6 

Rose-colored  urine;  no  albumen. 

7 

Normal  color;  no  albumen. 

g 

Rose-colored;  no  albumen. 

9 

Color  and  composition  normal. 

Total. 

6 

UNFAVORABLE. 

Prohibited  by  the  ordinance  of  the  police  commissioner  in  France.     (See  Lieber, 
p.  30.) 

Meyer  (J.  Amer.  Chem.  Soc.  1907,  v.  29,  pp.  900-901):  The  dog  experimented 
on  showed  signs  of  paralysis  on  the  morning  of  the  seventh  day  at  8  o'clock, 
and  died  at  10.40  a.  m.,  after  having  received  a  total  of  32  grams  of  color,  of 
which  1G  had  been  given  on  the  last  day.  The  initial  dose  was  70  grains  per 
100  pounds  body  weight;  the  total  weight  of  color  was  5,818  milligrams  per 
kilogram  body  weight,  or  4,073  grains  per  100  pounds;  the  average  dail] 
was  therefore  582  grains  per  100  pounds,  or  831  milligrams  per  kilogram  body 
weight. 

DOUBTFUL. 


1.  Winogradow  (Zts.  Xahr.  Genussm. 
inhibits  digestion, 


1903,  '.  5,  p.  689)  says  it  almost  completely 


G.  T.  65. 

Trade  names.—  Fael  Red  Bj  Bordeaux  I>:  Bordeaux  BL;  Bordeaux 
K  extra. 

Names  under  which  it  woe  offered  on  (lit   United  States  market  as  a 

d  color  in  1907*    Bordeaux  B;  Claret  lvc«i. 

Scientific  name.-— Alphanaphthj  Uanin-azo-betanaphthol-disulpho- 
oic  acid. 

Discovered.     1878. 

Shade.     Red.    Offered  by  2  out  <»f  L2  bout 


90  COAL-TAR   COLORS  VSED  IN    FOOD  PRODUCTS. 


FAVORABLE. 


1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  115):  " Bordeaux  Red  (Fast  Red  B)  not  poisonous  to  human  beings." 

3.  "Other  Azo  colors    *    *    *    Fast  Red  B    *    *    *    are  entirely  nonpoisonous." 

(p.  148.) 

4.  Fraexkel  (p.  575):  "That  the  monoazo  coloring  matters  examined  by  Cazeneuve 

and  Lepine,  as  already  above  stated,  are  nonpoisonous,  can  be  easily  explained 
by  the  constitution  of  these  substances.  These  two  investigators  examined 
*    *    *    Bordeaux  B." 

5.  Arloixg  and  Cazeneuve  (Archives  de  physiologie,  1887,  pp.  856-393):  As  a  result 

of  this  work,  which  is  divided  into  three  parts — (1)  Stating  the  effect  of  direct 
introduction  of  the  color  into  the  circulation;  (2)  intravenous  injections;  (3) 
comparing  the  effects  of  injections  of  color  and  of  salt;  and  (4)  feeding  by  the 
mouth — these  investigators  conclude  that  these  coloring  matters  are  toxic  only 
in  extremely  large  doses;  that  when  given  to  dogs  with  their  food  that  no  incon- 
venience of  any  kind  results;  this  is  based  upon  experiments  on  three  dogs, 
covering  145  days,  where  each  dog  received  per  kilogram  of  initial  body  weight 
in  the  first  case  20,307  milligrams,  or  14,213  grains  per  100  pounds  initial  body 
weight;  in  the  second  case,  29,590  milligrams,  or  20,713  grains  per  100  pounds 
initial  body  weight;  and  in  the  third  case,  28,154  milligrams,  or  19,758  grains 
per  100  pounds  initial  body  weight.  Per  day  this  means  98  grains  per  100 
pounds  initial  body  weight  in  the  first  case;  in  the  second  case,  143  grains  per 
100  pounds  initial  body  weight;  and  in  the  third  case,  137  grains  per  100  pounds 
initial  body  weight. 

6.  Cazeneuve  (Arch.  gen.  de  med.,  1886,  p.  753)  says  it  may  be  taken  without  effect 

by  man  or  animals,  sick  or  well,  in  large  doses. 

7.  Cazeneuve  and  Lepine  (Bull,  de  Vacad.  de  med.,  1886,  p.  643):  Tolerated  by  man 

well  or  sick. 

G.  T.  70. 

Trade  name. — Azarin  S. 

Scientific  name. — Ammonium    bisulphite    compound    of    dichloro- 
phenol-azo-beta-naphthol. 
Shade. — Red.     Not  offered. 


FAVORABLE. 


1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  115):  "Nonpoisonous    *    *    *    Azarin  S    *    *    *. " 

xperiments  on  five  dogs;  three  fed  by  the  mouth;  two  treated  hypodermically, 
of  which  latter  one  died.  The  first  dog  received  1,307  milligrams  per  kilogram 
body  weighl  in  25  days;  that  is,  54.7  kilograms  per  day  on  the  average,  or  a  total 
of  957  grains  per  100  pounds  of  body  weigh! ;  that  is,  38  grains  per  100  pounds 
body  weight  per  day.  The  Becond  dog  received  a  total  of  1,942  milligrams  ]>or 
kilogram  body  weighl  in  20  days,  orJ)7  milligrams  per  kilogram  body  weight  per 
day,  which  amounts  to  a  total  of  1,359  grains  per  LOO  pounds  body  weight,  or  68 

grains  per  I')')  pounds  body  weighl  per  day.  In  both  Cases  a  distinct  amount  of 
albumen  was  present  in  the  urine, and  the  urine 6 vol ved  sulphurous  acid  on  treat- 
ment  with  hydrochloric  acid.     The  third  dog  received  hypodermically  three 

do,-  in  eight  days,  each  dose  being  213  milligrams  per  kilogram  bodj  weight; 

that  i-.   I  19  '/mil!-  per  l<»"  pounds  body  Weight)   no  had  effects.     (/'•  !■■■■   I 

3.  "Administered  by  the  stomach  A/.arin  S  is  harmless."    (p.  134.) 

4.  " Other  Azo  colors,    *    *    *    for  instance  Azarin  8,  are  entirely  nonpoisonous. M 

(p.  148.) 

.',     PraBNKBL  \/.;irm  S  administered  hv  I  ho  stomach  i- entirely  harmless.  " 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 


91 


UNFAVORABLE. 

1.  Weyl  (p.  134):  Dog;  weight  not  given;  received  5  cc  of  Azarin  S  paste  by  injec- 

tion into  the  abdominal  cavity,  and  survived  three  days.  "The  cause  of  death 
was  considered  to  be  peritonitis  without  effusion.  The  result  of  this  post- 
mortem is  of  much  interest.  The  red  spots  consisted,  as  was  determined  by 
chemical  analysis,  of  the  azo  color  which  is  the  basis  of  the  Azarin  S.  Conse- 
quently in  the  peritoneal  cavity  the  same  splitting  up  of  the  Azarin  S  had 
occurred  which  takes  place  when  it  is  attached  to  textiles. " 

2.  Fraenkel  (p.  578):  To  the  same  effect. 

G.  T.  78. 

Trade  name. — Erika  B. 

Scientific    name. — Sodium    salt    of    methyl-benzen}Tl-amido-thio- 
xylenol-azo-alpha-naphthol-disulphonic  acid . 
Discovered  and  patented. — 1889. 
Shade. — Rose  Pink.     Xot  offered. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Chlopin  (p.  153) :  Based  on  his  own  experiments  considers  it  as  not  harmless.     The 
experimental  data  are  as  follows : 

Experimental  data  by  Chlopin. 
[1  gram=125  mg=87.5  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  ami  urine. 

1901. 
10 

Grams. 
2 

Kilos. 
8.0 

cc. 
392 
400 
120 
300 
390 
293 
J60 

no 

102 

880 

Dog  normal;  mine  add;  no  albumen. 

brine  of  rose  shade;  insignificant  traces  of  albumen;  acid. 

11 

Color  same;  no  albumen. 

12 

2 

Do. 

u 

Do. 

11 

Urine  vellow,  greenish  shade;  traces  of  albumen. 

15 

17 

2 

Do. 
Urine  wine  vellow,  orange,  acid;  DO  albumen. 

19 

Dog  quite  well;  urine  orange:  no  albumen. 

Total  . 

6 

G.  T.  84, 


Tradt    names. — Resorcin    Yellow;    Tropeolin    Oj    Trop®olin    K: 
Chrysoin;  Chiyseolin;  Yellow  T;  Gold  Yellow;  Acme  felloe  , 

Names  under  which  it  was  offered  on  the  United  States  market  as  q 

color  in  i'«>7.    Chrysoiii  REZj  Resorcio  0275. 
Scu  ntific  nam .    Sodium  Ball  of  para-eulphobenzene-azo-resorcinol. 
Discovered.     L875. 
Shadi .  —  Reddish  vellow.     Offered  by  2  out  of  12  sources. 


92 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


FAVORABLE. 

1.  Chlopin  {-pp.  131-2)  examined  this  color  physiologically,  and  has  classified  it  as 
harmless.    The  experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 

No.  l  (p.  M7). 

[1  gram=43  mg=30  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Apr.      9 
10 

Grams. 

Kilos. 
23.00 

cc. 
500 

Dog  quite  well;  urine  normal  color,  acid;  no  albumen. 
Do. 

11.21 
2  0.70 
12.00 

11 

Urine  acid;  no  albumen. 

12 

No  symptoms  of  poisoning;  eats. 
Urine  dark  brown;  no  albumen. 

13 

460 
520 
580 

14 

Do. 

17 

Urine  normal  color;  no  albumen;  dog  is  well. 

Total  . . 

13.21 
2  0.70 

No.  2. 
[1  gram=156  mg=109  grains.] 


1901. 
Oct.  9 
10 
11 
12 
13 
14 
15 
16 
17 
18 
19 
20 
21 
22-26 

Total... 


6.4 

30 
350 

2 
2 

300 
335 
290 
290 
375 
300 

2 

2 

2 

320 
360 
360 

7.0 

10 

Dog  well;  urine  yellow;  no  albumen. 

Do. 
Urine  brown,  acid;  no  albumen. 
Urine  light  brown,  acid;  no  albumen. 

Do. 

Do. 

Do. 

Do. 

Do. 

Do. 
Urine  light  brown,  acid,  no  albumen;  diarrhea. 
Brown  yellow,  acid,  no  albumen   no  diarrhea. 
Urine  normal;  dog  is  well. 

Do. 


1  Internally.  2  Subcutaneously. 

2.  Permitted  by  the  law  of  Italy. 

UNFAVORABLE. 

1.  Forbidden  by  the  Confectioners'  List. 

DOUBTFUL. 

1.  Winogradow  (Zts.  Nahr.  Genussm.,  1903,  v.  6,  p.  589)  says  it  noticeably  retards 
digestive  action;  not  indifferent. 

G.  T.  85. 

Tradenames. — Orangel;  Alphanaphthol Orange;  Naphl bo]  Orange; 
Tropseolin  OOO;  Orange  B. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1007. — Orange  KZ;  Orange  027. 

Scientific  name. — Sodium  salt  of  para-sulphobenzene-azo-alpha- 
oaphthol. 

Discovered, — 1876. 

Shade. — Orange.     Offered  by  2  out  of  12  sources. 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS.  93 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  31):  "According  to  Cazeneuve  and  Lepine's  experiments,  the  following 

are  not  poisonous  to  human  beings  and  dogs:     *    *    *    Orange     *    *    *." 

3.  "Orange  I  (Alpha-naphthol  Orange,  Tropaeolin  OOO)  not  poisonous  to  dogs  neither 

by  administration  by  stomach,  nor  by  injection  into  blood."  (On  authority  of 
Cazeneuve  and  Lepine.)     (p.  115.) 

4.  Weyl  {pp.  123,  148)  refers  to  this  as  not  poisonous. 

5.  Permitted  by  the  law  of  Italy. 

6.  Permitted  by  the  law  of  Austria. 

7.  Cazeneuve  (Arch.  gen.  de  med.,  1886,  Vol.  I,  p.  753)  says  it  may  be  taken  without 

effect  by  man  or  animals,  sick  or  well,  in  large  doses. 

8.  Cazeneuve  and  Lepine  (Bull,  de  I'acad.  de  med.,  1886,  p.  643):  Tolerated  by  man, 

well  or  sick. 

G.  T.  86. 

Tradenames. — Orange  II;  Betanaphthol  Orange;  Tropaeolin  000 
No.  2;  Mandarin  G  extra;  Chrysaurein;  Gold  Orange;  Orange  extra; 
Atlas  Orange;  Orange  A. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Xaphthol  Yellow  SLOZ;  Orange  II;  Orange; 
Orange  Y;  Mandarin  G  extra;  Orange  A  1201;  Orange  A  extra. 

Scientific  name. — Sodium  salt  of  para-sulphobenzene-azo-beta- 
naphthol. 

Discovered. — 1876. 

Shade. — Orange.     Offered  by  8  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  law  in  Italy. 

2.  Frentzel (Zts.  Nahr.  Genussm.,1901,  < .  4,  p. 974)  says  that  according  to  his  experi- 

ments this  color,  in  the  small  amounts  in  which  it  is  used  in  food  products  and 
which  can  enter  the  human  system  in  the  course  of  24  hours,  canhardh 
with  frequent  administration,  cause  a  harmful  affect 

3.  Frentzel  (Zts.  Nalir.Genussm.,  1901,  v.  4.  pp.  968-974)'-  Experimented  on  rabbits, 

giving  dye  with  food,  a  total  of  21  grams  in  19  days,  ■  total  of  S.748  milligram* 
per  kilogram  body  weight,  or  (i,  133  grains  per  100  pounds  body  weight,  in 
of  1  gram  each,  daily  for  the  first  15  days,  or  about  417  milligrams  per  kilogram 
of  body  weight,  or  292  grains  per  100  pounds  body  weight  pel  doae  far  these  L5 
doses;  the  color  could  only  l>e  detected   in  the  urine,  and  th<  •  came 

softer.  A  dog  was  given  i,o20  milligram!  per  kilogram  body  weight,  Of  714 
grains  per  loo  pounds  body  weight,  and  showed  distinct  kidney  irritation,  great 
thirst,  and  diarrhea;  recovery  required  about  one  week;  and  thereafter  the  same 

animal  was  fad  by  the  mouth  one-iw  ant  ieth  ol  the  above  d0S8  cadi  day  for  0 

Boccessh  e  days  without  any  untoward  effect ,  A  second  dog  recede  ed  per  kilo- 
gram of  body  weight  172  milligrams,  or  121  graini  per  LOO  pounds  body  weight, 

and   it,   like  the  lirst   dog,   in   tin-  first   experiment,  showed   kidney  irritation, 
diarrhea,  and  great   thirst.     <  >n  humans   K>0  milligrams,  or   U  grains,  colored 
the  urine  within  b">  minutes,  and  1  his  color  remained  far 24  hours;  there  1 
Sign  "f  Vomiting  or  diarrhea;  the  hitter  taMe  q|  the  COloi  1  able, 


94  COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

UNFAVORABLE. 

1.  Forbidden  by  Confectioners'  List. 

2.  Forbidden  by  Swiss  Analytical  chemists. 

3.  Wbtl  (p.  US):  "Poisonous  Orange  II.     *    *    *." 

4.  "  Betanaphthol  Orange  is,  therefore,  according  to  Experiment  I,  poisonous  in 

small  doses  when  administered  by  the  stomach,  and  suffices  to  kill  an  ordinarily 
large  strong  dog."     (p.  123) 

5.  A.  Weyl's  own  experiments  on  two  dogs,  the  initial  dose  in  one  case  being  476 

milligrams  per  kilogram  body  weight,  or  333  grains  per  100  pounds  body  weight; 
the  animal  receiving  in  the  course  of  20  days,  in  four  doses,  1,333  milligrams 
per  kilogram  body  weight,  or  933  grains  per  100  pounds  body  weight;  or  335 
milligrams  per  dose  per  kilogram  body  weight;  that  is,  225  grains  per  dose  per 
100  pounds  body  weight.  The  animal  died,  and  suffered  diarrhea  and  albumi- 
nuria, and  its  urine  was  colored  red  throughout  the  entire  period.  B.  The 
second  dog  received  hypodermically  per  kilogram  body  weight,  116  milligrams, 
or  61  grains  per  100  pounds  body  weight;  its  urine  was  colored;  albuminuria, 
diarrhea,  loss  of  hair,  abscesses,  and  loss  of  weight  occurred.  It  required  36 
days  to  recover  from  four  doses  administered  during  one  week.  C.  A  rabbit 
received  1,333  milligrams  per  kilogram  body  weight,  or  933  grains  per  100 
pounds  body  weight,  and  died  within  12  hours,     (p.  122) 

6.  "Of  the  23  Azo  colors  subjected  to  examination  only  two    *    *    *    Orange  II 

produce(s)  such  effects  when  administered  by  the  stomach  that  we  can  con- 
sider it  poisonous.  With  dogs  the  lethal  dose  is  less  than  1  gram  per  kilo  of 
the  body  weight  of  Orange  II    *    *    *."     (p.  147.) 

7.  "Further  Orange  II,  which  is  poisonous    *    *    V 

8.  "The  poisonous  qualities  of  Orange  II." 

9.  "Further,  in  spite  of  the  presence  of  the  sulpho  groups,  colors  may  be  poisonous, 

as  is  shown  with  Orange  II."     (p.  148.) 

10.  Chlopin  (Zts.  Nahr.  Genussm.,  1902,  v.  5,  p.  241):  A.  A  dog  received  349  milli- 

grams per  kilogram  body  weight,  or  244  grains  per  100  pounds  body  weight  for 
the  first  day  of  experiment,  which  dose  was  repeated  on  the  third  and  fourth 
days;  nothing  untoward  is  noted  for  the  first  three  days  in  the  condition  of  the 
dog;  the  urine  was  dark  red  but  free  from  albumen;  on  the  fifth  and  sixth  days 
two-thirds  of  the  above  amount  was  given,  and  on  the  seventh  and  eighth  days 
the  original  dose  was  given.  On  the  fourth  day  the  animal  was  frisky  and  had 
a  good  appetite  but  was  vomiting;  on  the  fifth  day  vomiting  stopped,  but 
diarrhea  ensued,  which  diarrhea  continued  for  one  week;  the  weight  remained 
practically  constant;  the  urine  was  colored  throughout  from  dark  red  to  orange 
red  and  dark  brown  and  became  normal  the  fourth  day  after  the  last  ad  mi  nisi  ra- 
tion. B. Humans:  Chlopin  took  200  milligrams,  or  3^  grains,  in  a  gelatin  capsule 
at  3  p.  m.;  at  4.30  p.  m.  the  urine  was  colored  a  strong  red  orange;  at  6  p.  in. 
a  dryness  of  throat  and  bad  taste  in  mouth  appeared;  at  6.30  p.  m.  felt  very 
badly;  vertigo  and  unable  to  remain  seated  and  continue  writing;  blood  rushed 
to  head;  tin-  general  condition  very  poor;  somewhat  improved  by  moving 
about  in  open  air;  7.30  felt  so  poorly  took  (dauber's  -alt  as  an  antidote;  II  |».  m. 
ill  condition  still  continuing;  urine  normal  yellow;  midnight  recovered. 

Chlopin  states  that  he  would  not   repeal    this  experiment   on  himself,  or  on 
any  other  human,  and  he  concludes  therefore  that   this  color  must  he  regarded 

as  harmful. 

11.  CnLOPiN  (p.  1.33)  (dasses  it  as  "harmful."     The  experimental  data  are  as  follows: 


COMPILED    DATA    UNDER    GREEX    TABLE    NUMBERS. 


95 


Experimental  data  by  Chlopin. 
[1  gram=116mg=81  grains.] 


Date. 


Weight. 


24-hours 
urine. 


General  condition  of  animal  and  urine. 


1901. 

May  27 

28 

29 

30 

31 
June  1 
2 
3 
4 
5 


Total.. 


Grams. 


Kilos. 
8.6 


8.2 


8.59 


Dog  is  quite  well;  urine  normal. 
Urine  brown  red,  acid;  no  albumen. 

Do. 
Diarrhea  and  vomiting  at  night,  no  albumen;  urine  orange  red, 

acid,  no  albumen. 
Diarrhea  continues;  no  albumen;  no  vomiting. 
Diarrhea  continues;  dog  lively,  eats  with  relish;  no  albumen. 
Urine  brown  orange,  acid,  no  albumen;  diarrhea  continues. 
Urine  clear;  no  albumen;  diarrhea  continues. 
Urine  dark  brown;  no  albumen;  diarrhea  decreases. 
Diarrhea  still  less:  no  albumen. 

Diarrhea  very  slight;  urine  Slightly  orange,  no  albumen. 
Urine  normal  in  color  and  composition;  diarrhea  stopped. 


12.  Buss  lists  it  as  poisonous. 

DOUBTFUL. 

1.  Winogradow  (Zts.  Xuhr.  Genussm.,  1903,  v.  6,  p.  5S9)  says  it  almost  completely 
inhibits  digestion. 

G.  T.  87. 

Trade  names. — Orange  III;  Ilolianthin;  Tropaeolin  D;  Methyl 
Orange;   Dimetlivl.-milin  Orange. 

Scientific  name. — Sodium  salt  of  para-sulphobenzene-azo-diniethy- 
lanilin. 

Discovered. — 1876. 

Shade. — Orange  Yellow.     Not  offered. 

FAVORABLE. 

1.  Permitted  by  the  law  of  Italy. 

IN  FAVORABLE. 

1.  Chlopin  (pp.  145,  146)  on  his  own  experiments  classes  it   as  poisonous.     The 
experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 
No.  1. 
[1  gram  =  l(V{  mg  =  114  grains.] 


'     "Trim'"' 


General  condition  of  animal  :m<l  i irin.>. 


Sept. 


1901. 


M 

M 
1 
2 
:< 

■» 
5 

7 


Grams. 


Kilns. 


<> 

6b  U 

310 



805 

•J 

a 

Total  .. 


10 


Before  experimenl  dog  quite  normal;  color  urine  usual,  add, 
no  albumen. 
Do. 
Color  of  urine  dark  yellow;  no  albumen. 
Urine  brown;  reddish  with  sulpburio  add;  no  albumen. 

Do. 
Do. 
Urine  dark  brown;  no  albumen;  vomit 

dog  does  not  eat,  but  drinks  with 
Complete  ataxia,  which  became  general  on  the  9th;  dog  can  do! 
move  tn  straignt  line,  and  wa 
on  tl  lis;  after  Calling  arises  with  difficulty  and 

with  widely  spread  feet,  continuously  lifting  r 
then  the  other;  extremii  on  11th  days  I 

cultv;  placed  on  his  feet,  maintained  equilibrium  with  dif- 
ficulty: involuntarily  H  1  moves  it  about  in  the 
air;  animal  can  stlU  swallow;  i  I  to  light;  d 

id  the  L2th  the  hind  legs  completelj   |  on  the 

ltth  vomiting  ::■  of  the  fro:  •  quietly 

without  moving;  La  kill  .  shows  no  change  in  Lri- 

i  i  in  the  lumbar  repion  of  th<> 

■  .1  column  (?)  borderinj  nterior  and  Lateral 

columns,"  causing  death  by  paralysis  of  the  heart. 


96 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Experimental  data  by  Chlopin — Continued. 

No.  2. 

[1  gram=149  mg= 104.3  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Dec.       3 

Grams. 
3 

Kilos. 
6.7 

cc. 

A  few  hours  after  giving  color  dog  in  tremors;  does  not  eat. 
Urine  black;  acid;  no  albumen;  paralysis  of  the  extremities. 
Dog  lies  in  cage  in  full  paralysis;  died  "before  dinner;  no  albu- 
men in  urine;  cause  of  death,  paralysis  of  heart. 

4 

Little. 
Little. 

2.  Meyer  (J.  Amer.  Chem.  Soc,  1907,  v.  29,  p.  900):  Dog  receiving  113  milligrams 

per  kilogram  body  weight;  that  is,  79  grains  per  100  pounds  body  weight.  Result, 
diarrhea,  which  continued  throughout  17  days,  although  only  3  doses  of  the 
same  size  were  given  in  6  days;  thereafter  the  dose  was  increased  geometrically; 
the  diarrhea  continued;  the  coloring  matter  was  discharged  in  the  urine  and 
the  feces;  there  was  no  abnormal  condition  revealed  by  the  autopsy. 

DOUBTFUL. 

1.  Winogradow  (Zts.  Nahr.  Genussm.,  1903,  v.  6,  p.  589)  says  it  noticeably  retards 
digestive  action;  is  not  indifferent. 

G.  T.  88. 

Trade  names. — Diphenylamin  Orange;  Orange  IV;  Tropseolin  00; 
Orange  M;  Fast  Yellow;  Orange  G  S;  New  Yellow;  Orange  N;  Acid 
Yellow  D. 

Scientific  name. — Sodium  salt  of  para-sulphobenzene-azo-diphenyl- 
amin. 

Discovered. — 1876. 

Shade. — Orange  Yellow.     Not  offered. 

FAVORABLE. 

1.  Weyl  (p.  115):  "Nonpoisonous    *    *    *     Diphenylamin  Orange    *    *    * 
2    *    *    *    Diphenylamin  Orange  is    *    *    *    nonpoisonous."     (p.  132.) 

3.  "For  instance,  the  poisonous  Metanil  Yellow  corresponds  to  the  nonpoisonous 

Diphenylamin  Orange."     (p.  148.) 

4.  The  experiments  on  which  Weyl  based  the  conclusions  above  may  be  summarized 

as  follows:  A.  A  dog  received  183  milligrams  per  kilogram  body  weight,  or 
128  grains  per  100  pounds  body  weight.  The  urine  was  rendered  black,  and 
contained  traces  of  phenol  and  abundant  albumen;  this  condition  lasted  for 
72  hours,  at  the  end  of  which  110  milligrams  per  kilogram  body  weight,  or 
77  grains  per  100  pounds  body  weight,  were  administered;  urine  became 
colorless  and  albumen  diminished.  Five  days  afterwards  a  total  of  10  grams, 
or  366  milligrams  per  kilogram  body  weight,  or  256  grain-  per  100  pounds 
body  weight,  were  administered;  the  urine  became  abundant,  was  strongly 
black,  alkaline,  contained  albumen.  The  loss  qJ  freight  was  1  kilogram,  or 
about  3$  percent.  B.  A  dog  received  308  milligrams  per  kilogram,  or  216  grains 
per  LOO  pounds  body  weight,  as  the  initial  dose;  albuminuria  did  not  result 
until  after  repeated  dosing  same  ai  initial  dose,  and  administered  for  2  weeks. 

5.  Weyl'.-    conclusions    arc    as    follows:  "According    to    (he    above    investigations, 

Diphenylamin  Orange  causes  albuminuria,  but  further  disturbances  did  not 

appeal  during  the  Beveral  weeks'  observations  on  the  animals  used," 


COMPILED   DATA    UNDER    GREEN    TABLE    NUMBERS. 


97 


6.  Chlopin  (p.  148)  examined  this  color  and  classes  it  as  nonpoisonous.     The  ex- 
perimental data  are  as  follows : 

Experimental  data  by  Chlopin. 

[1  gram=145  mg=100  grains.] 


Date. 

Dose. 

WdtfJ  "Jgf 

General  condition  of  animal  and  urine. 

1901. 
Oct.    27 
28 

Grams. 
3 

Kilos. 

7 

cc. 
300 

Dog  quite  normal;  urine  color  normal;  no  albumen. 
Urine  dark  brown;  acid;  no  albumen. 

Do. 

Do. 

Do. 
Urine  yellow,  with  sulphuric  acid  red;  no  albumen. 
Orange  with  orange  sheen;  no  albumen. 

Do. 
Urine  brown  vellow:  acid:  no  albumen. 

29 

3 
3 
3 
3 
3 
3 

30 

31 

Nov.    1 

2 

340 

3 

G.5 

4 

275 

5 

3 

300             Do. 

6 

6.7 

Do. 

Total. 

24 

7.  Fraenkel  (pp.  577,  578)  to  the  same  effect  as  Weyl,  as  above. 

8.  Permitted  by  the  law  of  Italy. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

G.  T.  89. 

Trade  names. — Brilliant  Yellow  S;  Yellow  WR;  Curcumin. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907.— Brilliant  Yell.  >w  S. 

Scientific  name. — Sodium  salt  of  para-sulphobenzenc-a/.o-diphenyl- 
amin-suphonic  acid. 

Shade. — Yellow.     Offered  by  1  out  of  12  source-. 

1 AVORABLE. 

1.  Lieber  (p.  136):  A  very  young  rabbit  received  ,-ix  doses  on  alternate  days, 

doae  amounting  to  320  milligrams  per  kilogram  of  body  weight,  or  22 1  grains  per 
100  pounds  of  body  weight.  No  untoward  symptoms  arc  recorded;  the  body 
vreight  increased  almost  10  percent  in  11  da 


Nothing. 


i \ ! A\ ORABLE. 


G.  T.  92 


Tradi   minus.     Ax<>  Acid  Yellow;  A/«>ila\in:  Azo  Yellow;  Indian 
Yellow. 
Scientific  name.     Mixture  of   nitrated   diphenylamin  yellow  with 

nit  n>-diplieii\  lamin. 
Piston  in/.       I^so. 

sIkk/i  .     Yellow.     Not  offered. 

•  1°     Hull.  117—12 7 


98 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


FAVORABLE. 

1.  Chlopin  (p.  128)  examined  this  color  and  classifies  it  as  nonpoisonous.     The  ex- 
perimental data  are  as  follows: 

Experimental  data  by  Chlopin. 

No.  l. 

[1  gram=125mg=87.5grains.] 


Date. 

Dose. 

Weight. 

urine^  I                       General  condition  of  animal  and  urine. 

1901. 
Apr.     6 
8 

Grams. 
2 

Kilos. 
8 

cc. 
370 

Little. 

Dog  normal;  urine  acid;  no  albumen. 
Urine  reddish  orange;  acid;  no  albumen. 
Do. 

10 

3 

11 

600 
430 

Urine  red;  no  albumen. 

12 

Urine  almost  normal  color;  acid;  no  albumen. 

Total  . 



5 

Conclusion:  Nonpoisonous. 


No.  2  (p.  129). 
[1  gram=  143  mg=  100  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Apr.   12 
14 

Grams. 
2 
3 

Kilos. 

7 

cc. 
430 
610 
600 
400 

Dog  normal;  urine  acid;  no  albumen. 
Do. 

15 

Urine  dark  vellow;  acid;  no  albumen. 

16 

Urine  almost  normal  color;  acid;  no  albumen. 

Total.. 

5 

Conclusion:  Showed  no  harmful  effects. 
2.  Permitted  by  law  in  Italy. 

UNFAVORABLE. 

Nothing. 

DOUBTFUL. 

1.  Winogradow  (Zts.  Nahr.  Genussm.,  1903,  v.  6,  p.  589)  says  it  almost  completely 
inhibits  digestion;  noticeably  retar.l-  digestive  action;  is  not  indifferent. 

G.  T.  93. 

Trade  name. — Azo-fuchsin  G. 

Scientific   name. — Sodium    salt    of    para-sulphobenzene-azo-dioxy- 
naphthalene-sulphonic  acid. 
Discovered. — 1880. 
Slwde. — Reddish  brown.     Not  offered. 


FAVORAHLK. 


l    Chlopin  (pp  1  >>.  i  7)  examined  this  color  and  classifies  it  as  nonpoisonous.    The 
experimental  data  an-  at  foil* 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 

Experimental  data  by  Chlopin. 
No.  1. 
[1  gram=117  mg=  82  grains.] 


99 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901 
May     3 

Grams. 
2 

Kilos. 
8.5 

cc. 
300 
363 
390 
380 

285 

420 
292 

Dog  well  and  normal;  urine  acid;  no  albumen. 
Urine  chocolate  brown;  acid;  no  albumen. 

5 

2 

Do. 

6 

Urine  dark  brown,  chocolate,  in  thin  layer  greenish  sheen;  acid; 

no  albumen. 
Urine  slightly  greenish;  acid;  no  albumen. 

7 

2 

8 

Dark  chocolate  brown;  acid;  no  albumen. 

9 

8.7 

Urine  normal;  dog  is  well. 

Total. 

6 

No.  2. 
[1  gram=125mg=  87.5  grains.] 


1901. 
Oct.      9 

8.0 

390 
310 

10 

2 
2 

11 

12 

380 
325 

13 

2 

14 

15 

2 

2 

396 

16 

17 

397 
325 
380 
246 
420 

18 

2 

19 

20 

21 

8.4 

Total. 

12 

Dog  quite  normal;  urine  acid;  no  albumen. 

Do. 
Urine  slightly  more  yellow;  no  albumen. 
Urine  dark  brown;  acid;  no  albumen. 

Do. 

Do. 

Do. 

Do. 

Do. 

Do. 
Urine  almost  black;  acid;  no  albumen. 
Urine  almost  black;  acid;  no  albumen;  urine  of  lighter  color. 

Do. 


Nothing. 


UNFAVORABLE. 


DOUBTFUL. 


1.  Winogradow  (Zts.  Nahr.  Genussm.,  1903,  v.  6,  p.  589)  says  it  almost  completely 
inhibits  digestion. 

G.  T.  94. 

Trade  names. — Tartrazin;  Hydrazin  Yellow. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Flavazein  Red  Shade  Z;  Tartrazin;  Acid  Yel- 
low AT. 

Scientific  name. — Sodium  salt  of  benzcne-azo-pyrazalone-caiboxv- 
disulphonic  acid. 

Discovered. — 1884. 

shade. — Yellow.    Offered  l>y  6  <>ut  of  L2  lources. 

DOUBTFUL. 

1.  Lieber  (p.  134):  Dog,  2  months  old,  received,  pet  kilo,  body  weight,  :'.:  milli- 
gram-, <>r  26  gnim  per  i<><>  pounda  body  weight,  -ix  rimon  on  alternate  day* 

The  animal  sul'lVrod    (TOO)   mild   diarrhea  at    the  .-tart,   which  Continued   with 
greater  or  less  activity  than  at  tin- -tart  throughout  thot<-t. 


100  COAL-TAR    COLORS   USED   IX    FOOD   PRODUCTS. 

2.  Meyer  {J.  Amer.  Chem.  Soc,  1907,  v.  29,  p.  897):  Dog  received  100  milligrams 
per  kilogram  body  weight,  or  70  grains  per  100  pounds,  increased  in  geometric 
proportion  for  6  consecutive  days,  at  the  end  of  which  time  diarrhea  set  in. 
On  that  day  2,000  milligrams  per  kilogram  body  weight,  or  1,400  grains  per  100 
pounds  body  weight,  were  administered;  this  was  about  two-thirds  as  much  as 
the  animal  had  received  in  all  the  5  days  preceding;  the  feces  were  colored 
after  the  first  administration,  and  the  urine  was  also  colored;  albuminuria 
doubtful. 
3.  Fraenkel  (pp.  210  and  216):  Tartrazin,  according  to  the  Green  Tables,  is  a 
derivative  of  isopyrazolon;  "*  *  *  only  those  substances  which  are  deri- 
vatives of  pyrazolon  are  antipyretics,  the  isopyrazolon  derivatives  are,  how- 
ever, poisonous."  Tartrazin  is  also  closely  related  to  the  antipyrin  class  of 
compounds,  which  class  is  known  to  possess  an  irritant  action  and  also  a  de- 
pressing action  on  the  circulation.  Tartrazin  also  contains  benzol  groups, 
which  are  said  to  increase  the  physiological  activity  of  pyrazolon  derivatives. 

G.  T.  95. 

Trade  names. — Metanil  Yellow;  Orange  MN;  Tropaeolin  G. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Victoria  Yellow  cone.  Z;  Yellow  MXX  cone. 

Scientific  name. — Sodium  salt  of  meta-sulphobenzene-azo  diphenyl- 
amin. 

Discovered. — 1 8  7 (.  I . 

Shade. — Orange.     Offered  by  2  out  of  12  sources. 

FAVORABLE. 

1.  Frentzel  (Zts.  Nahr.  Genussm.,  1901,  v.  4,  p.  974):  A.  A  rabbit  received  379 

milligrams  per  kilogram  body  weight,  or  265  grains  per  100  pounds  body  weight; 
no  color  administered  for  2  days,  and  then  administered  at  intermittent  periods, 
so  as  to  receive  6  doses  in  19  days.  Total  weight  administered  per  kilogram 
body  weight  2,085  milligrams,  or  1,400  grains  per  100  pounds,  whieli  is  equivalent 
to  77  grains  per  day  per  100  pounds;  the  color  could  always  be  detected  in  the 
urine,  and  the  feces  became  softer.  B.  A  dog  received  581  milligrams  per 
kilogram  body  weight  at  one  dose;  that  is,  407  grains  per  100  pounds  body  weigh! . 
There  was  no  vomiting  and  no  diarrhea;  the  dye  persisted  in  the  urine  for  72 
hours.  C.  The  same  dog,  after  recovering  from  the  foregoing,  received  daily 
one-tenth  the  above  dose  for  9  days;  the  dyestufi  was  found  in  the  urine  and  the 
feces  and  movements  were  normal;  dissection  showed  nothing  abnormal. 
I».  A  human  swallowed  loo  milligrams,  or  L.g  grains;  no  untoward  symptomi 
are  recorded;  tin-  urine  remained  colored  for  24  hours.  From  the  foregoing 
Pren'tzel  Concludes  that  this  coloring  matter  is  absolutely  harmless. 

2.  Chlopin  [Zti.  Nahr.  Qenuttm.,  A.  A  dog  received  305  milli- 

•  ,   per  kilogram  body  weight;  thai  is,  L04  grains  per  LOO  pounds  body  weight; 

no  color  administered  for  four  days;  the  same  dose  was  given  on  alternate  days 

mx  times,  and  the  dose  was  increased  60  per  cent,  and  that  dose  administered 
twice,  and  the  original  dose  was  given  on  the  next  alternate  day;  altogether  the 
animal  received  per  kilogram  body  weight,  3,355  mUligrams,  or  1,144  grains 
per  LOO  pounds  body  weight,  in  i  period  of  22  days,  or  an  average  o!  153  milli- 
gram! per  kilogram  body  weight  per  day,  or  52  grains  per  day  per  LOO  pounds 
body  weight.  Ai  tie-  end  of  the  twelfth  day  albuminuria  set  In,  and  it  required 
throe  m  i  k    iftei  <  et  ing  the  administration  of  the  color  for  the  albuminuria 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 


101 


2.  Chlopin  (Zts.  Nahr.  Genussm.,  1902,  v.  5,  p.  241 )— Continued. 

to  disappear;  the  urine  was  colored  throughout  the  period  of  dosing,  and  it  was 
not  until  10  days  after  the  last  color  had  been  administered  that  the  urine 
regained  normal  color;  otherwise  the  animal  was  well  throughout.  B.  Hu- 
mans: Two  hundred  milligrams,  or  3-T2  grains  taken  at  3  p.  m.,  October  30, 
1901,  colored  the  urine  so  highly  yellow  that  it  could  be  dyed  with.  Apart 
from  the  bitter  taste  of  the  product  no  untoward  symptoms  are  recorded.  C. 
Chlopin's  conclusion  {Zts.  Nahr.  Genussm.,  1902,  v.  5,  p.  244)'-  "Metanil  Yellow 
is  not  poisonous  to  dogs  in  doses  of  from  2  to  3  grams  per  day,  nor  to  humans 
in  doses  of  0.2  grams  per  day,  and  may  therefore  perhaps  be  regarded  as  non- 
poisonous  from  a  practical  point  of  view." 

UNFAVORABLE. 

1.  Weyl  (p.  115):  "Poisonous    *    *    *    Metanil  Yellow." 

2.  Says  the  product  smelled  strongly  of  diphenylamin.     (/;.  ISO.) 

3.  A.  "Metanil  Yellow  must  be  considered  poisonous  when  administered  by  the 

stomach  from  the  indications  of  Experiments  1  and  2.  The  lethal  dose,  which 
is  determined  by  Experiment  2,  is  0.53  grams  per  kilo  body  weight."  This 
lethal  dose  is  371  grains  per  100  pounds  body  weight.  B.  A  dog  received  862 
milligrams  per  kilogram  body  weight,  or  603  grains  per  100  pounds  body  weight. 
This  caused  vomiting;  the  same  dose  was  repeated  24  hours  afterward.-*,  the 
animal  again  vomiting.  The  animal  died  within  96  hours  from  the  first  admin- 
istration. C.  A  dog  received  89  milligrams  per  kilogram  body  weight,  or  62 
grains  per  100  pounds  body  weight;  the  urine  became  colored  about  96  hours 
after  administration;  5  days  after  the  first  administration  the  animal  was  given 
10  times  the  original  dose;  vomiting  set  in  within  one  hour;  in  24  hours  the 
urine  was  deeper  colored;  a  week  later  after  the  dose  last  preceding,  one-half 
of  that  dose  was  given,  and  the  animal  died  within  24  hours;  the  animal  had 
lost  during  this  period  approximately  one-quarter  its  original  weight,     (p.  182.) 

4.  "*    *    *     Metanil  Yellow    *    *    *    produce[s]  such  effects  when  administered 

by  the  stomach  that  we  can  consider  them  [it]  poisonous."     (p.  147.) 

5.  "The  poisonous  qualities  of      *    *    *    Metanil  Yellow;  the  poisonous  Metanil 

Yellow."     (p.  148.) 

6.  Fraexkel  (p.  578):  "A  dog  weighing  11  kilograms  was  killed  by  20  grams  of 

this  coloring  matter  within  four  days,  whereas  the  isomeric  Diphenylamin 
Orange  is  nonpoisonous,  and  it  must  first  be  considered  if  the  poisonous  nature 
of  this  substance  can  be  explained  by  the  easy  liberation  of  diphenylamin 
from  it,  since  this  coloring  matter,  in  and  of  itself,  ha- a  strong  odor  of  diphenyla- 
min." 

7.  Chlopin  (p.  141)'-  Based  on  his  own  experiments  considers  it  "Not  quite  harm- 

fas."     The  experimental  data  arc  as  follows: 

imental  data  fry  chlopin. 

[1  Kram      153  XQg      In?  grains.] 


D  ito. 

Weight. 

M  boars' 

urine. 

(.fin r.il  <  cm  id  it  ion  <>f  animal  and  urine. 

1901. 

M.r.     Lfl 
1  | 

cc. 
ISO 

100 

370 

(  rine  unusual  color;  acid;  no  albumen. 
Do 

20 

21 

I'rii  ■                          1;  DO  albumen. 

Do 

Do 

24 

B0 

25 

M 

2 

27 

102 


COAL-TAR   COLORS   USED   IN   FOOD  PRODUCTS. 
Experimental  data  by  Chlopin — Continued. 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
May  28 
29 

Grams. 
2 

Kilos. 

cc. 
330 
350 
350 
355 
400 
340 
330 
400 
305 
390 
330 
335 

Do. 

30 

2 

Do. 

31 

Do. 

2 

2 

Do.                                                     * 

3 

Do. 

4 

3 

Do. 

5 

Do. 

6 

3 

Do. 

7 

Do. 

8 

2 

Do. 

9-29 

6.5 

Color  of  urine  normal  June  18,  on  29th  albumen  disappears.  Dog 
is  well. 

Total. . 

22 

8.  Chlopin  (p.  141)'-  On  authority  of  others  not  stated,  classes  this  color  as  harmful 

or  poisonous. 

9.  Prohibited  by  the  laws  of  Italy. 

10.  Prohibited  by  Confectioners'  List. 

11.  Prohibited  by  the  Resolutions  of  the  Society  of  Swiss  Analytical  Chemists,  Sep- 

tember, 1891. 

12.  Buss  lists  it  as  poisonous. 

DOUBTFUL. 

1.  Winogradow  {Zts.  Nahr.  Genussm.,  1903,  v.  6,  p.  589)  says  that  it  noticeably 
retards  digestion. 

G.  T.  97. 

Trade  names. — Orange  T;  Mandarin  G  R;  Orange  R;  Kermesin 
Orange. 

Name  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Orange  2  R. 

Scientific  name. — Sodium  salt  of  sulpho-ortho-toluene-azo-beta- 
naphthol. 

Shade. — Orange.     Offered  by  1  out  of  12  sources. 


Nothing. 


FAVORABLE. 
UNFAVORABLE. 


1.  Chlopin  {p.  125):  Based  on  his  own  experiments  considers  this  color  as  "harm- 
ful."    The  experimental  data  are  as  follows: 

No.  l. 


D:ii.-. 

1  >■<  '■. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  vim. 

1901. 
Apr.     4 

Grams. 

Kilos. 

cc. 

310 
280 
420 
570 

:i7o 

an 

330 

Nothing  abnormal. 

Urine  reddish  brown;  traces  of  albumen;  acid. 

6 

3 

Do. 

7 

I'rine  dark  brown;  acid;  traces  of  albumen. 

H 

Color  of  urine  weaker;  no  albumen. 

9 

Almost   normal-colored   urine;  no   albumen;  dog   is   well  and 

10 

liwly. 
Nothing  abnormal. 

Total.. 

4 

COMPILED  DATA  UNDER   GREEN   TABLE   NUMBERS. 

No.  2. 
[1  gram  =  217  mg  =  152  grains.] 


103 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1902. 
Jan.    25 

26 

Grams. 
2 

Kilos. 
4.6 

cc. 
200 

Soon  after  giving  color  heavy  vomiting  and  diarrhea:  dog  does 

not  eat  or  drink  the  rest  of  the  day;  urine  acid;  no  albumen. 
Vomiting  and  diarrhea  continued;  dog  is  tired  and  run  down, 

27 

and  began  to  eat;  urine  dark  brown  and  no  albumen. 
Urine  same;  dog  livelier. 

28 
29 

2 
2 

4.3 

180 
200 

Diarrhea  and  vomiting  stopped;  urine  of  brown  color;  acid;  no 

albumen. 
Urine  orange;  no  albumen;  acid. 

Total.. 

6 

G.  T.  102. 

Trade  names. — Fast  Red ;  Roccellin ;  Cerasin ;  Rubidin ;  Fast  Red 
A;  Rauracienne;  Orcellin  No.  4. 

Scientific  name. — Sodium  salt  of  para-sulphonaphthalene-azo-beta- 
naphthol. 

Shade. — Brownish  red.     Not  offered. 

Discovered  and  patented. — 1877. 

FAVORABLE. 

1.  Permitted  by  the  law  of  Italy. 

2.  Permitted  by  the  law  of  Austria. 

3.  Cazeneuve  (Arch.  gen.  de  mtd.,  1886,  p.  753)  says  it  may  be  taken  without  effect 

by  man  or  animals,  sick  or  well,  in  large  dot 

4.  Cazeneuve  and  Leplne  (Bull,  de  Vacad.  de  mcd.  1886,  p.  643):  Tolerated  by  man 

well  or  sick. 

G.  T.   103. 

Trade  names. — Azorubin  S;  Carmoisin;  Azo  Acid  Rubin;  Fast  Red 
C;  Azorubin  A. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Claret  Red  RZ;  Cardinal  3  B;  Azorubin;  Car- 
moisin B. 

Scientific  name. — Sodium  salt  of  para-sulphonaphthalene-azo- 
alpha-naphtbol-para-sulphonic  acid. 

Discovered  and  patented. — 1883. 

Shade. — Red.     Offered  by  6  ou1  of  12  sources. 


I  AVnli.MI!  |, 

Permitted  by  Confectionera'  List. 

Cazknkivi;  am»  I.i  iinj  :   Not  poJSODOUl  t"  human  frflinm 

Meyek  (./.  Anur.   Chun.  S,,c.  One  hundred  milligrams  mr 

kilogram  body  weight,  <<r  70  grains  pef  km)  pounds  body  weight  adminktered, 
increased  geometrically;  diarrhea  wei  marked  only  after  edminietrati 
exceptionally  large  doaei  (the  leventh  day;  the  stools  were  deep  viol 
the  urine  irai  carmine,  becoming  dark;  the  autopsy  developed  nothing  abnor- 
mal; the  Whole  interior  was  of  a  red  Color. 


104 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


4.  Lie  be  r  (p.  138):  A  guinea  pig  received  once  a  day  six  times  every  other  day 
241  milligrams  per  kilogram  body  weight,  or  169  grains  per  100  pounds  body 
weight;  appetite  remained  good  throughout,  and  aside  from  an  occasional 
thirstiness  noted  no  untoward  observations  were  recorded. 

G.  T.  105. 

Trade  names. — Fast  Red  E;  Fast  Red. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1 907 .— Claret  Red  RZ. 

Scientific  name. — Sodium  salt  of  para-sulphonaphthalene-azo-beta- 
naphtkol-monosulphonic  acid . 

Discovered  and  patented. — 1878. 

Shade. — Red.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Meyer  (J.  Amer.  Chem.  Soc.  1907,  v.  29,  p.  898):  Initial  dose  100  milligrams  per 

kilogram  body  weight  or  70  grains  per  100  pounds,  and  given  three  times 
increased  geometrically  once  before  diarrhea  was  observed;  there  was  no 
albumen  in  the  urine;  urine  was  colored  deep  red;  feces  colored  red  at  the 
start,  at  the  end  of  the  experiment  chocolate  brown;  autopsy  showed  all  parts 
to  be  substantially  normal. 

3.  Cazeneuve  and  Lepine   (Compt.   rend.,  1885,   v.   101,  pp.  823-827):  A.   Dog: 

Weight  21.5  kilo,  received  as  follows: 


Days. 

Grams. 

Milligrams 
par  kilo. 

Grains  per 
100  pounds. 

32 

20 

8 

10 

0.500 
2.150 
4.300 
5.  000 
10.000 

23.2 
100.0 
200.0 
232.  0 
402.0 

16.2 

70.0 
140.0 
1 62.  0 

324.  0 

Nothing  abnormal  except  occasional  greenish  urine;  no  vomiting;  no  diarrhea. 
B.  Man:  1.  One  of  the  experimenters  took  1  gram,  dissolved  in  wine,  daily 
for  15  days;  no  effect.  2.  A  man  aged  25,  afflicted  with  albuminuria,  received 
the  following: 


Crams. 

3 
2 

1 

ii  5 
I  0 

ed  colic  without  diarrhea;  amount  oi  urine  or  albumen  not  affected.  3. 
Three  men  afflicted  with  Blight's  disease  received  each  daily  for  8  days  I  gram; 
no  effect  on  the  albumen,  l.  A  30  year-old  man  chronic  invalid  took  l  grama 
one  day,  6  grams  the  next  day;  do  effect  was  observed. 


COMPILED  DATA  UNDER  GREEN   TABLE    NUMBERS.  105 

4.  Arloing  and  Cazeneuve  (Archives  de  physiologie,  1887,  pp.  356-393):  As  the 
result  of  this  work,  which  is  divided  into  four  parts:  (1)  Stating  the  effect  of 
direct  introduction  of  the  color  into  the  circulation;  (2)  intravenous  injections; 
(3)  comparing  the  effects  of  injections  of  color  and  of  salt;  and  (4)  feeding  by 
the  mouth — these  investigators  conclude  that  these  coloring  matters  are  toxic 
only  in  extremely  large  doses;  that  when  given  to  dogs  with  their  food  no 
inconvenience  of  any  kind  results;  this  is  based  upon  experiments  upon  three 
dogs,  covering  145  days,  where  each  dog  received,  per  kilogram  initial  body 
weight,  in  the  first  case,  20,307  milligrams,  or  14,215  grains  per  100  pounds 
initial  body  weight;  in  the  second  case,  29,590  milligrams,  or  20,713  grains 
per  100  pounds  initial  body  weight;  in  the  third  case,  28,154  milligrams,  or 
19,758  grains  per  100  pounds  initial  body  weight.  Per  day  this  would  mean  98 
grains  per  100  pounds  initial  body  weight  in  the  first  case;  in  the  second  case 
the  daily  dose  was  143  grains  per  100  pounds  initial  body  weight;  and  in  the 
third  case  the  daily  dose  was  137  grains  per  100  pounds  initial  body  weight. 

G.  T.  106. 

Trade  names. — New  Coccin;  Cochineal  Red  A;  Brilliant  Scarlet; 
Crocein  Scarlet  4  BX. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Claret  Red  RZ;  Crocein  Scarlet;  Xew  Coccin; 
Scarlet  L;  Brilliant  Scarlet  4  R. 

Scientific  name. — Sodium  salt  of  para-sulphonaphthalene-azo-beta- 
naphthol-disulphonic  acid  (G.). 

Discovered. — 1878.     Offered  by  5  out  of  12  sources. 

Shade. — Red. 

FAVORABLE. 

1.  Cazeneuve  and  Lkpine.     (See  Weyl,  p.  115.) 

2.  Weyl  (p.  31):  "*     *    *     not  poisonous   to  human  beings  and   dogs,      *     *     * 

Purple    *     *    *" 

3.  Cazkxeuve  and  Lepine  (Bull,  de  Vacad.  de  mid.,  t886t  p.  W  '■  Tolerated  by  man. 

sick  or  well. 

INI AVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

G.  T.  107. 

Tradenames. — Fasi  Red  D;  Azo  Acid  Rubin  2  B;  Fast  Red  E  Bj 
Bordeaux  S;  Amaranth. 

Names  under  which  if  was  offered  <>n  tin    United  State*  market  ■ 
food  color  in  1907.     Claret   Red  RZ;  Red;  Amaranth  B  (Azo  color 
similar  to) ;  Bordeaux  S;  Naphthol  Red  S;  Amaranth. 

Scientific  name.  Sodium  Bali  <»f  para-8ulphonaphthalene->azo-beta- 
naphthol-disulphonic  acid  (R). 

Discovered  and  /><if>  nt<</.     is?v 

Shade.     Red.     Offered  l>\  7  <>ut  <>f  12  souro 


106  COAL-TAR   COLORS  USED  IN   FOOD  PRODUCTS. 

FAVORABLE. 

1.  Cazeneuve  and  Lepine  (see  Weyl,  p.  115):  Not  poisonous  to  human  beings. 

3.  Lieber  (p.  148):  A  rabbit  received  284  milligrams  per  kilogram  body  weight,  or 

199  grains  per  100  pounds  once  a  day,  five  times  every  other  day,  and  aside  from 

decreased  appetite  the  second  and  third  day  of  the  observation  period  nothing 

untoward  is  noted. 
4    Weyl  {p.  31):  "*    *    *    not  poisonous  to  human  beings  and  dogs,     *    *    * 

Purple    *    *    *" 
5.  Cazeneuve  and  Lepine  (Bull  de  Vacad.  de  mid.,  1886,  p.  648):  Tolerated  by  man, 

sick  or  well. 

G.  T.  138. 

Tradenames. — Fast  Brown  G;  Acid  Brown. 

Scientific  name. — Sodium   salt  of   bi-sulphobenzene-disazo-alpha- 
naphthol. 

Discovered. — 1882. 

Shade. — Brown.     Not  offered. 

FAVORABLE. 

1.  Weyl  (p.  134):  "The  following  is  a  summary  of  the  results  obtained  with  the  Dis- 
azo  colors  submitted  to  test  by  me,  viz,  Fast  Brown  G  *  *  *.  All  these 
proved  to  be  nonpoisonous  *  *  *."  A.  A  dog  weighing  9.63  kilos  received 
312  milligrams  per  kilogram  body  weight,  or  218  grains  per  100  pounds  body 
weight;  the  same  dose  was  repeated  48  hours  afterwards,  when  diarrhea  set  in, 
and  the  urine  was  colored  red ;  24  hours  afterwards  208  milligrams  per  kilogram 
body  weight,  or  146  grains  per  100  pounds  body  weight  were  given;  the  urine 
was  colored  strongly  red  24  hours  thereafter.  Eight  days  afterwards  520  milli- 
grams per  kilogram  body  weight,  or  364  grains  per  100  pounds  body  weight,  were 
administered ;  marked  diarrhea  set  in;  3  days  later  the  dose  given  was  twice  the 
dose  last  given,  when  severe  diarrhea  resulted,  but  unchanged  color  appeared  in 
the  urine,  and  continued  for  24  hours  afterwards ;  diarrhea  continued  for  96  hours. 
Evidences  of  albuminuria  apparently  not  dependable.  B.  A  second  dog, 
weighing  5.9  kilos,  received  339  milligrams  per  kilogram  body  weight,  or  237 
grains  per  100  pounds  body  weight  daily  throughout  an  entire  month;  diarrhea 
was  produced  after  6  days,  which  continued  almost  during  the  month;  appetite 
was  diminished  and  the  loss  in  weight  was  about  20  per  cent  on  the  original. 
C.  Weyl  concludes  as  follows:  "According  to  these  experiments,  this  color 
in  continuous,  though  slight,  doses,  or  in  large  doses,  but  less  frequently, 
produces  diarrhea,  anorexia,  and  emaciation."     (p.  136.) 

unfavorable. 

1.  Prohibited  by  Confectioners'  List. 

2.  Weyl  (p.  147):  "Of  the  remaining  colors    *     *     *    others  (produce)  diarrhea 

(Fast  Brown     *    *     *)." 

G.  T.  160. 

Trade  name. — Crocein  Scarlet  3  B;  Ponceau  4  RB. 
Scientific  name. — Sodium  salt  of  sulphobenzene-azo-benzene-azo- 
beta-naphthol-monoeulphonic  add. 

Discovered  and  yatented. — 1881. 
Shade. — Scarlet.     Not  offered. 


COMPILED  DATA  UNDER   GREEN   TABLE    NUMBERS.  107 

FAVORABLE. 

Nothing. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

DOUBTFUL. 

1.  Houghton  (/.  Amer.  Chem.  Soc,  1907,  v.  29,  pp.  1351-57):  Hinders  fibrin  diges- 
tion at  all  strengths;  at  1: 200  hinders  casein  and  albumen  digestion. 

G.  T.  163. 

Tradenames. — Biebrich  Scarlet;  Ponceau  B;  New  Red  L;  Ponceau 
3  RB;  Fast  Ponceau  B;  Imperial  Scarlet. 

Scientific  name. — Sodium  salt  of  sulphobenzene-azo-sulpho-ben- 
zene-azo-beta-naphthol. 

Discovered. — 1878. 

Shade. — Scarlet.     Not  offered. 

FAVORABLE. 

1.  Permitted  by  law  in  Italy.     (See  Licber,  pp.  18,  22,  23.) 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

G.  T.  164. 

Trade  name. — Crocein  Scarlet  O  extra. 

Scientific  name. — Sodium    salt    of    sulphobenzene-azo-sulphoben- 
zene-azo-beta-naphthol-sulphonic  acid. 
Discovered. — 1888. 
Shade. — Scarlet.     Not  offered. 

FAVORABLE. 

Nothing. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

G.  T.  166. 

Trade  name. — Wool  Black. 

Scientific  name. — Sodium    salt    of    sulpliobenzeiu'-uzo-sulphohen- 
zene-azo-para-tolvl-bcta-naplitliylainin. 
Discovered. — 1885. 
Shade. — Black.     Not  offered. 

I    \\  "KAMI   1 

1.  Permitted  by  ( Sonlectioners'  List 

2.  Wkyi.  (y.  //;■:  "The  following  Is  a  summary  "f  the  reeulti  obtained  with  the 

Disa/o  colon  submitted  to  teet  l>y  me,  viz:  *    *    *    Wool  Back    *    *    *. 

All  thete  proVrd   to  h«-   IloM])(>isonOU8      *      *      *." 


108  COAL-TAR   COLORS  USED   IX   FOOD  PRODUCTS. 

3.  A.  A  dog  received  167  milligrams  per  kilogram  body  weight,  or  117  grains  per 
100  pounds  body  weight  each  day  for  3  successive  days;  no  color  was  admin- 
istered for  the  next  2  days,  and  the  third  day  the  dose  was  double  the  former 
dose.  The  urine  was  colored  bluish-black  and  contained  albumen.  Two  days 
afterward  the  same  dose  was  given;  urine  of  intense  dark-blue  color,  and  con- 
tained unaltered  coloring  matter,  which  disappeared  in  48  hours.  Albuminuria 
continued  for  about  15  days.  (p.  137.)  13.  "Wool  Black  is  nonpoisonous  both 
by  gastric  and  by  subcutaneous  administration."     (p.  137.) 

G.  T.  169. 

Trade  names.  —  Crocein  Scarlet  7  B;  Ponceau  6  RB;  Crocein 
Scarlet  8  B. 

Xames  under  which  it  was  offered  on  the  United  States  market  as  a 
food-color  in  1907. — Sodium  salt  of  sulphotoluene-azo-toluene-azo- 
beta-naphtliol-alpha-sulphonic  acid . 

Discovered  and  patented. — 1881. 

Shade. — Red.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

G.  T.  188. 

Trade  names. — Naphthol  Black  B;  Brilliant  Black  B. 

Name  under  which  it  was  offered  on  the  United  States  market  as  a  food- 
color  in  1907  —  Naphthol  Black  BDF. 

Scientific  name. — Sodium  salt  of  disulpho-beta-naphthalene-azo- 
alpha-naphthalene-azo-beta-naphthol-disulphonic  acid. 

Discovered  and  patented. — 1885. 

Shade. — Black.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  Li<t . 

2.  Weyl  (p.  138):  A.  A  dog  received  112  milligrams  per  kilogram  body  weight,  or 

78  grains  per  100  pounds  body  weight,  daily  for  3  successive  days;  distinct 
albuminuria,  uncolorod  urine;  blue-colored  feces;  thereupon  the  daily  dose  was 
increased  to  L87  milligrams  per  kilogram  body  weight,  that  is,  131  grains  per 
L00  pounds.  No  color  was  administered  for  o  days,  and  during  this  time  the 
urine  was  colored  from  reddish-violet  to  a  bluish-black  red;  thereupon  the  last 
doubled  and  'i  \  hours  afterwardfl  that  dose  was  doubled;  rather  much 

albumen  in  urine  which  was  bluish;  albuminuria  continued  for  about  a  week. 

B.  A  dog  received  222  milligrams  per  kilogram  body  weight,  or  155  grains  per 
loo  pounds  daily throughoul  a  whole  month;  it  remained  entirely  well  with 

:  appetite. 

3.  "This  color  is  harmless  when  administered  by  the  stomach,  but  poisonous  sub- 

<  otaneousl)  "    (p    I 

4.  Bchachbbl:  Not  harmful  under  conditions  in  which  if  is  used. 

I    \  I  A  \  oKAHI  I    . 

l  \\'i:Yi.(j>.  tS9)\  Where  a  dog,  receiving  subcutaneously  81  milligrams  per  kilogram 
body  weight,  or  22  grains  per  LOO  pounds  body  weight]  subcutaneously,  died 
apparently  wholly  us  :i  result  of  the  color. 


COMPILED  DATA  UNDER  GREEN   TABLE    NUMBERS.  109 

2.  "Naphthol  Black  P,  however,  is  plainly  poisonous  when  introduced  into  the  sub- 
cutaneous cellular  tissue."     (p.  147.) 

G.  T.  197. 

Trade  names. — Bismarck  Brown;  Phenylene  Brown;  Leather 
Brown;  English  Brown;  Manchester  Brown;  Vesuvin;  Cinnamon 
Brown. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food-color  in  1 907 . — Vesuvin  4B  Cone.  Z;  Bismarck  Brown;  Bismarck 
Brown  B  No.  216;  Bismarck  Brown  B. 

Scientific  name. — Hydrochloric  1  of  benzene-disazo-phenylene^liamin, 

Discovered  and  patented. — 1863. 

Shade. — Reddish  brown.     Offered  by  4  out  of  12  sources. 

FAVORABLE. 

1.  Weyl  (p.  115):  " Nonpoisonous  Bismarck  Brown." 

IN!  AVIIHAHI  V  . 

1.  Prohibited  by  Confectioners'  List. 

2.  Wbtl  (p.  117):  A.  A  dog  received  33  milligrams  per  kilogram  body  weight,  or 

23  grains  per  hundred  pounds  body  weight ;  in  one  and  one-half  hours,  vomiting; 
next  day  BBme  dose  same  result  with  the  addition  that  the  animal  took  no  food 
and  moved  about  but  little  for  48  hours;  on  the  fourth  day  same  dose,  in  two 
hour-,  vomiting;  for  9G  hours  animal  took  no  food;  on  the  eighth  day  albumen 
in  the  urine  and  the  animal  ate;  on  the  ninth  day  83  milligrams  per  ki! 
body  weight  or  58  grains  per  100  pounds  body  weight,  vomited  for  one-half  hour 
after  administration;  for  the  next  5  days  the  animal  took  hardly  any  food;  on 
the  fourteenth  day  the  animal  improved,  took  food  on  the  fifteenth  day;  tra 
albumen  in  urine  for  17  days  longer,  at  end  of  which  time  animal  recovered. 
B.  A  dog  received  L69  milligrams  per  kilogram  body  weight,  or  L18  grains  per 
100  pounds  body  weight;  in  24  hours  the  urine  was  colored  brown;  48  hours 
after  the  first  dose  that  dose  was  repeated,  and  unconverted  color  was  found 

in  the  urine;  48  hours  later  the  same  dose  was  repeated;  the  color  in  the  urine 
disappeared   in  24  hours;  4  days  later  the  dose  W8S  trebled,  and  the  animal 

vomited,  Beemed  sick  for  4  days  thereafter;  on  the  fifth  day  reco\  cry  apparently 
complete.    On  the  sixth  day  the  Last  dose  was  repeated,  and  the  animal  vomited 

after  tin-  administration.      It   took  QO  food   for  24  hours,  and   was  normal  after 

48  hours.    There  was  uo  albuminuria  in  this  ca 
0.  A  dog  received  daily  for  an  entire  month  45  milligrams  per  kilogram  bod] 
pht,  or  31)  graini  per  LOO  pounds  body  weight;  it  was  in  good  health  during 

the  entire  time,  did   not    vomit,   and  at€  M  usual.      Its  gaio  in  weight    I 

per  cent . 

3.  "Bismarck  Brown  produces,  when  administered  I  the  itomach,  even 

in  <!  0  milligrams  per  kilogram  body  wei  grains  per  i<x)  pounds 

body  weight  ,  vomiting  and  albuminuria.    Further  disturbance  is  not  noted 

even  in  1  ;  small  doses,    1"»  milligrams  per  kilogram  l>odv  weight  (or 

:J1J  grains  p»-r  L00  pounds  body  weight),  eveo  when  frequently  admim 
seem  to  be  entirely  barmle  t.     Doses  of  L6  milligrams  are  harmless  even  when 
introduced  into  the  subcutaneous  cellular  tissue  "    (p.  tI8.) 

4.  "Of  the  remaining  colon  some  produce   vomitii  .    Bismarck    Brown 


110        COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

5  Lewix  (Lehrbuch  der  Toxikologie.  1897,  p.  231):  Produces  eczema,  and  cites 
Deutsch  Med.  Wochenschr. t  1891,  p.  45. 

6.  Fraexkel  (p.  575):  "When  the  Azo  dyestuffs  do  not  contain  any  sulpho  group 
they  are  poisonous.  Thus,  for  example,  Bismarck  Brown  *  *  *.  This 
produces  no  effect  in  email  doses;  on  the  other  hand,  doses  of  350  milligrams 
per  kilogram  of  animal  (245  grains  per  100  pounds)  produce  albuminuria  and 
vomiting." 

DOUBTFUL. 

1.  Houghton*  (/.  Amer.  Chem.  Soc,  1907,  v.  29,  pp.  1351-1357):  Hinders  digestion 
of  fibrin,  casein  and  albumen,  in  strengths  of  1:100  or  1:400. 

G.  T.  201. 

Trade  names. — Manchester  Brown  EE;  Bismarck  Brown  R; 
Vesuvin  B. 

Names  under  which  it  was  offered  on  the  Vnited  States  market  as  a 
food  color  in  1907 . — Vesuvin  4  B  Cone.  Z;  Vesuvin  B. 

Scientific  name. — Hydrochloric!  of  toluene-disazo-meta-tolylene- 
diamin. 

Discovered  and  patented. — 1878. 

Shade. — Reddish  brown.     Offered  by  2  out  of  12  sources. 

UNFAVORABLE. 

1.  Lewix  (Lehrbuch  der  Toxicologic,  1S97,  p.  231):  "Produces  eczema,"  and  cites 
Deutsch.  Med.  Wochenschr.,  1891,  p.  45. 
Note. — The  literature  is  not  always  conclusive  as  between  Nos.  197  and  201,  and 
probably  most,  if  not  all,  the  references  under  No.  197  also  apply  to  No.  201. 

G.  T.  240. 

Trade  name. — Congo  Red. 

Name  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Congo. 

Scientific  name. — Sodium  salt  of  diphenyl-disazo-binaphthionic 
acid. 

Discovered  and  patented. — 1884. 

Shade. — Red.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Weyl:  "According  to  Experiments  1  and  2  Congo  Red  is,  after  long-continued 

administration  by  the  stomach,  harml- 

2.  A.  A  dog  received  274  milligrams  per  kilogram  body  weight,  or  192  grains  per  100 

pounds ;  this  dose  was  repeated  next  day,  when  the  urine  became  pale,  was  strongly- 
alkaline  and  contained  albumen;  the  next  day  the  same  dose  was  repeated, 
whereupon  the  urine  was  of  a  weak  red  color,  and  a  little  albumen  present; 
the  next  day  the  dose  was  increased  to  411  milligrams  per  kilogram  body 
-  grains  per  100  pounds;  the  urine  was  somewhat  reddish  and  con- 
tained a  little  albumen.  No  color  was  given  for  6  days,  at  the  end  of  which 
time  the  urine  was  reddish,  and  deposited  i  reddufa  sediment,  probably  Congo. 
At  the  end  of  that  time  the  dose  was  increased  to  685  milligrams  per  kilogram 


COMPILED   DATA  L'NDEE   GREEN    TABLE    NUMBERS.  Ill 

2.  A. — Continued. 

body  weight,  or  480  grains  per  100  pounds  body  weight;  the  urine  was  feebly 
alkaline  and  contained  some  albumen.  The  next  day  the  dose  last  given  was 
doubled;  the  urine  was  colored  to  such  an  extent  that  it  could  be  dyed  with. 
Two  days  later  the  same  dose  was  repeated;  animal  took  but  little  food,  wa3 
otherwise  comfortable;  there  was  little  albumen  present.  The  loss  in  body 
weight  was  about  A.\  per  cent.  (p.  141.) 
B.  A  second  dog  received  233  milligrams  per  kilogram  body  weight,  or  163  grains 
per  100  pounds,  daily  for  one  month,  and  remained  entirely  well. 

G.  T.  269. 

Trade  name. — Chrysamin  R. 

Xame  under  which  it  v:as  offered  on  the   United  States  market  as  a 
food  color  in  1907. — Chrysamin  R. 

Scientific  name. — Sodium  salt  of  ditolyl-disazo-bisalicylic  acid. 

Discovered  and  patented. — 1884. 

Shade. — Yellow.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  134  :  "The  following  is  a  summary  of  the  results  obtained  with  Disazo 

colors  submitted  to  test  by  me,  viz:  Chrysamin  R."  "AD  of  these  proved 
to  be  nonpoisonous,    *    *    *.*' 

3.  A.  A  dog  received  515  milligrams  per  kilogram  body  weight,  or  361  grains  per 

100  pounds;  urine  became  alkaline  and  yellowish,  and  easily  dyed  cotton; 
very  little  albumen.  Within  24  hours  the  same  dose  was  repeated,  diarrhea 
resulting  and  vomiting  for  3  days,  whereupon  the  animal  was  given  one-fifth  of 
the  dose,  or  103  milligrams  per  kilogram  body  weight,  that  is,  72  grains  per  100 
pounds  body  weight;  the  urine  continued  slightly  colored,  and  contained  a 
distinct  amount  of  albumen,  continuing  for  2  days,  when  the  last  dose  was 
repeated;  24  hours  afterwards  the  dose  was  doubled,  and  repeated  the  next 
day;  the  day  after  the  dose  was  increased  50  per  cent;  3  days  later  the  last 
dose  was  repeated;  slight  albuminuria  set  in,  lasting  5  days.  B.  A  dog  received 
three  doses  of  619  milligrams  each  per  kilogram  body  weight,  or  433  grains  per 
100  pounds  body  weight,  three  times  in  the  course  of  10  days;  the  urine  was 
yeUowiflh  in  color  and  contained  very  little  albumen,     (p.  145.) 

4.  "Chrysamin  is  harmless  when  taken  into  the  stomach 

5.  Schacherl  (p.  :  Chrysamin  is  harmless  under  the  conditions  in  which 

it  is  used. 

UNFAVORABLE. 

1.  WlTL(p.  U  ^he  remaining  colors  some  produced   vomiting    *     *     ■ 

others  diarrhea  (*    *     *    Chrv.-uniin  R    *    *    *.") 

G.  T.  277. 

Trade   names. — Benzopurpurin    4    B:   Cotton     Red     4     B;    Sultan 
Red  4  B. 

8c%efUi)  ■  . — Sodium  >alt  of  dit<>lvl-di-az<>-l>inaplitlii<>nic  acid. 

Discovered,     l^i  B5. 
8hadi .     Red.     No!  offered. 


112 
Nothing. 


COAL-TAK  COLORS  USED  IN  FOOD  PRODUCTS. 

FAVORABLE. 
UNFAVORABLE. 


1.  Chlopin  {p.  130):  On  his  own  experiments  classes  it  as  suspicious.     The  experi- 
mental data  are  as  follows: 

Experimental  data  by  Chlopin. 
[1  gram=125  mg=87.5  grains.] 


General  condition  of  animal  and  urine. 


Date. 

Dose. 

Weight. 

24-hour 
urine. 

1901. 
Apr.   16 
17 

Grams. 
2 

Kilos. 
8 

cc. 
300 
330 
450 
470 
370 
320 
310 
370 
310 

18 

3 

19 

20 

21 

2 

22 

23 

24 

Total. 

7 

Dog  is  well,  lively;  urine  normal  color;  acid;  no  albumen. 

Do. 
Vomiting  several  times;  no  albumen. 
Urine  yellow-orange;  no  albumen;  no  vomiting. 

Do. 

Do. 

Do. 
Urine  normal;  dog  is  well. 

Do. 


DOUBTFUL. 

1.  Winogradow  (Zts.  Nahr.  Genussm.  1903,  v.  6,  p.  589)  says  it  almost  completely 
inhibits  digestion. 

G.  T.  287. 

Trade  name. — Azo  Blue. 

Name  under  which  it  was  offered  on  the  United  States  market  as  a  food 
color  in  1907. — Azo  Blue. 

Scientific  name. — Sodium  salt  of  ditolyl-disazo-bi-alpha-nuphthol- 
para-sulphonic  acid. 

Discovered. — 1 885. 

Slvade. — Grayish  violet.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  I  p.  tS4)i  The  following  is  a  summary  of  the  results  obtained  with  the  Disazo 

colors  submitted  to  test  by  me,  viz:  *  *  *  Azo-blue,  *  *  *  ."  ''All 
these  proved  to  be  nonpoisonous." 

3.  "Azo-blue  Lb  harmless,   both  when  administered  by  the  stomach  and  subcuta- 

oeously.'i  A.  A  dog  received  237  milligrams  per  kilogram  body  weight,  or  166 
graina  per  LOO  pounds;  2  days  later  this  same  dose  was  repeated,  and  the  urine 
was  a  \i<»ict  color  strongly  alkaline  ami  contained  a  little  albumen.  The  next 
day  tie-  dose  was  increased  to  2.5 times;  colorless  urine,  and  little  albumen; 
there  was  do  phenol.    'The  next  day  I  I  imee  the  original  dose  was  administered; 

abundant    bluish-violet    urine  and    little  albumen.     No  administration   for  4 

<\.r.  i,  when  2.5  times  the  original  dose  wen  given,  and  that  d<>so  repeated  3  days 

later;  during  this  time  ihe  urine  was  colorless  and  contained  little  albumen; 

there  was  a  very  slight  increase  in  weight.  B.  A  dog  received  319  milligrams 
per  kilogram  body  weight,  or  233  grains  per  100  pounds  daily  Cor  one  month; 
animal  remained  well  with  good  appetite;  a  slight  amount  of  albumen  made 
its  appearance  in  the  urine,    (p.  144.) 


COMPILED  DATA  UXDER   GBEKN    TABLE    NUMBERS.  113 

UNFAVORABLE. 

1.  Weyl  (p.  144)'  "A  slight  amount  of  albumen  made  its  appearance  in  the  urine. " 

G.  T.  394. 

Trade    names. — Dinitrosoresorcin;  Dark    Green;    Russian    Green; 
Alsace  Green;  Fast  Green  O;  Chlorin;  Fast  Myrtle  Green. 
Scientific  name. — Dinitroso-resorcinol  (Dioximidoquinone). 
Discovered  and  patented. — 1875. 
Shade. — Green.     Not  offered. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  63):  "  According  to  the  above  experiments  Dinitroso-resorcinol  is  not 

dangerous  to  dogs  when  administered  by  the  stomach  even  in  large  doses; 
while  hypodermic  administration  proves  fatal  within  24  hours,  in  the  proportion 
of  190  milligrams  per  kilogram  of  body  weight"  (that  is,  132  grains  per  100 
pounds). 

3.  A.  A  dog  received  173  milligrams  per  kilogram  body  weight,  or  121  grains  per  100 

pounds;  scanty  dark-brown  urine;  the  next  day  the  same  dose  was  repeated  and 
urine  continued  dark  brown,  and  contained  trace  of  albumen  as  well  as  distinct 
reaction  for  iron;  the  next  day  the  dose  was  repeated;  animal  remained  lively; 
the  day  after  that  the  dose  was  increased  50  per  cent;  no  albumen.  The  1< SB  in 
body  weight  was  only  4  per  cent.  B.  A  dog  received  19S  milligrams  per  kilo- 
gram body  weight,  or  139  grains  per  100  pounds;  seems  to  have  been  loss  of 
appetite,  coupled  with  dark-brown,  almost  black  urine;  2  days  later  the  d>  - 
doubled,  and  the  urine  was  colored  green  by  ferrous  oxid,  and  contained  no 
albumcTi  nor  sugar;  2  days  later  the  dose  was  increased  50  per  cent,  and  some 
albumen  was  then  found  in  the  urine,     (p.  62.) 

G.  T.  398. 

Trade  name. — Naphthol  Green  B. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Naphthol  Green;  Naphthol  Green  B. 

Scientific  name. — Ferrous  sodium  salt  of  nitroso-betanaphthol- 
beta-monosulphonic  acid. 

Discovered. — 1883. 

Shade. — Green.     Offered  by  2  out  of  12  sources. 

•  >K  Mi!   I 

l.  Wsyl(ji  '■  ■  \  A  dog  received  172  milligrams  per  kilogram  body  weight,  or  120 
graini  i"-r  loo  pounds  body-weight;  the  arise  wat  greenish,  and  conjunctiva 
stained  intensely  green;  repeated  -\  successive  days,  and  the  next  day 

the  dose  was  increased  to  fivefold;  appetite  undisturbed,  and  animal  remained 
lively.     B.  A  dog  received  417  milligrams  per  kilogram  body  weight, 
grains  per  100  pounds;  there  was  •  dirty  yellowish-green  color  to  the  urine;  do 

albumen,  and  OOi   more  than  tnces  Ol  iron.     'The  animal  was  normal  within  a 

day,  and  two  days  after  the  same  repeated;  do  change  in  animal  was 

recorded,  except  that  on  tin-day  following  the  feces  were  normal,  but  colored 

•  en 

I]       Bull.  L47  -12 8 


114  COAL-TAR   COLORS  LTSED   IN   FOOD   PRODUCTS. 

2.  Weyl  (p.  65):  "Experiments  1  and  2,  in  which  2  to  5  grams  of  the  color  were  intro- 

duced directly  into  the  stomach,  demonstrated  its  harmlessness  in  this  method 
of  administration." 

3.  Buss  lists  it  as  nonpoisonous. 

UNFAVORABLE. 

1.  Prohibited  by  Confectioners'  List. 

2.  Weyl  (p.  65):  "On  the  other  hand,  in  a  hypodermic  administration,  in  two  out  of 

three  cases  abscesses  and  septic  fever  were  induced." 

G.  T.  399. 

Trade  names. — Sun  Yellow;  Curcumin  S;  Jaime  Soleil;  Maize. 
Scientific  name. — Sodium  salt  of  the  so-called  Azoxy-stilbene-disul- 
phonic  acid. 

Discovered. — 1883. 

Shade. — Yellow.     Not  offered. 

FAVORABLE. 

1.  Meyer  (J.  Amer.  Chem.  Soc,  1907,  v.  29,  p.  897):  A  dog  received  100  milligrams 
per  kilogram  body  weight,  or  70  grains  per  100  pounds,  increased  geometrically 
through  the  fourth  day,  when  diarrhea  set  in;  up  to  this  time  the  animal  had 
been  given  19.27  grams,  or  1,465  milligrams  per  kilogram  body  weight,  equiv- 
alent to  1,026  grains  per  100  pounds  body  weight;  the  average  dose  per  day 
would  have  been  366  milligrams  per  kilogram  body  weight,  or  256  grains  per 
100  pounds;  the  animal  was  given  its  fifth  portion  of  coloring  matter  the  same 
size  as  the  fourth,  thereupon  color- was  omitted,  and  for  the  following  7  days  the 
dosage  of  the  third  day,  which  amounted  to  400  milligrams  per  kilogram  body 
weight,  or  280  grains  per  100  pounds  body  weight,  was  given;  the  urine  was  col- 
ored orange  throughout  the  entire  test  after  the  first  day;  the  fecal  matter  also 
was  of  orange  color;  slight  diarrhea  on  the  fourth  and  twelfth  days  of  the  test, 
and  vomiting  on  the  fifth  day,  the  cause  of  which  does  not  seem  to  have  been 
definitely  determined;  the  autopsy  revealed  nothing  abnormal. 

G.  T.  425. 

Trade  names. — Auramin;  Auramin  O;  Pyoctanin  Aureum. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Auramin  O;  Auramin;  Canary  Yeilow. 

Scientific  name. — Ilydrochlorid  of  Lmido-tetramethyl-diamido- 
diphenylmethane. 

Discovered. — 1883 . 

Shade. — Greenish  yellow.     Offered  by  '•*>  out  of  L2  sources. 


Nothing. 


I   \\  OB  A  HI  I   . 


i   NFAVORAB1  I 


I.  Chlopin  (p.  tS7):  On  his  own  experiments  classes  i1  m  poisonous.    The  experi- 
mental data  are  aa  follows: 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 

Experimental  data  by  Chlopin. 
[1  gram =09  mg=48  grains.] 


115 


Date. 

Dose. 

Weight. 

24-hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Mar.  2-4 
6 

Grams. 
1.0 

Kilos. 
14.4 

cc. 
550 
340 

Dog  quite  normal;  acid;  no  albumen. 

Urine  strong  brown  yellow;  traces  of  albumen;  appetite  less. 

Thin  stool. 

7 

8 

Diarrhea;  urine  brown  yellow,  pales  with  sulphuric  acid,  and 

contains  much  albumen. 
Stool  normal;  color  of  urine  weaker;  much  albumen;  eats  well; 

9 

10 

lively. 
Stool  normal;  urine  less  colored;  less  albumen. 

11 

335 

Stool  normal;  urine  less  colored;  traces  of  albumen. 

12 

Stool  normal;  urine  less  colored;  insignificant  traces  of  albumen. 

13 

Do. 

14 

2.0 

13.2 

Do. 

15 

Strongly  brown  yellow;  much  albumen. 

Dog  depressed;  lies  down;  eats  little. 

Vomits  and  diarrhea;  urine   strong   yellow;  little   albumen; 

takes  only  milk. 
Vomits  and  diarrhea;  urine  strong  vel low;  much  albumen. 

16 

None. 
295 

480 

17 

19 

20 

Feces  normal  color;  color  urine  almost  normal;  much  albumen. 

21 

352 

380 

Feces  normal  color;  color  urine  almost  normal;  albumen  less. 

24 

10.4 

13.6 

Do. 

1  Subcutaneously. 

DOUBTFUL. 

1.  Winogradow  (Zts.  Xahr.  Genussm.,  1903,  v.  6,  p.  589)  says  it  noticeably  retards 
digestive  action;  is  not  indifferent. 

G.  T.  427. 

Trade  names. — Malachite  Green;  New  Green;  Fast  Green;  Benzal 
Green;  Diamond  Green  B;  Malachite  Green  B;  New  Victoria  Green; 
Vert  Diamant;  Bitter-almond-oil  Green. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Green  M;  New  Green  Crystals;  Green  088. 

Scientific  name. — Zinc  double-chlorid,  oxalate,  ferric  double-chlorid 
of  tetramethyldi-para-amido-triphenyl-carbinol. 

Discovered. — 1877-78. 

Shade. — Bluish  green.     Offered  by  2  out.  of  12  sources. 

I  AVOKAI1I.K. 

1.  Permitted  by  Confectioners'  List. 

2.  W'i^i.  "According  i<>  Gmndhomme    *    *    *    Malachite  Green  are  |  is) 

;il-<>  Qonpoisonous." 

3.  "*    *    *    Malachite  Green  are  (is)  as  is  now  established,  almost  without  poison' 

<>ii-  action."    (p.  55.) 
•i.  I.i  ui\  {Lehrbuch  (It  'V<>r'ik<>h><;  ays  when  free  from  arsenic  it  is 

harmless. 
.">    Buss  list    M  ;i-  iionp 

ONI  4VORAB1  i 

1     l'i\/ i     .1'        -  r,„r.  path,  phnrm.,   !  ( >n<«  hundred  in  ill  i- 

grams  per  kilogram  body  weight  o!  rabbit,  or  70  grams  per  100  pounds,  injected 
subcutaneously,  caused  after  the  third  day  motor  paralysifl  and 
cramps,  which  resulted  fatally  at  tin-  end  of  the  ninth  day. 


116 


COAL-TAR    COLORS   1TSED   IN    FOOD   PRODUCTS. 


2.  Lewin  (Lehrbuch  der  Toxihologie,  1897,  p.  231):  In  the  case  of  one  workman,  in 
contrast  with  others  who  had  long  been  unaffected  by  this  substance,  itching, 
burning,  inflammation,  and  swelling  of  hands  and  feet,  and  formation  of  blisters 
occurred. 

G.  T.  428. 

Trade  names. — Brilliant  Green;  New  Victoria  Green;  Emerald 
Green;  Malachite  Green  B;  Ethyl  Green;  Fast  Green  J. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907 . — Green  E;  Green  087;  Emerald  Green  Crystals. 

Scientific  name. — Sulphate  of  zinc-double-chlorid  (rarely  oxalate) 
of  tetraethyl-diamido-triphenyl-carbinol. 

Discovered.— 1879-80. 

Shade. — Yellowish  green.     Offered  by  3  out  of  12  sources. 

FAVORABLE. 

1.  Lewin  (Lehrbuch  der  Toxikologie,  1897,  p.  231)  says  when  free  from  arsenic  it  is 

harmless. 

2.  Buss  lists  it  as  nonpoisonous. 

UNFAVORABLE. 

1.  Chlopin  (pp.  171-2):  Classifies  it  as  "very  poisonous"  on  his  own  experiments 
(see  p.  181).     The  experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 

No.  1. 
[1  gram=125  mg=87.5  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Apr.      24 
25 

Grams. 

Kilos. 
8 

cc. 
410 

Before  experiment  dog  is  well;  urine  normal. 

2 

Soon  after  giving  dye  vomiting  and  diarrhea;  in  the  evening 

26 

395 

only  drank  water;  vomiting  kept  up. 
No    vomiting;  urine    greenish;  acid;  insignificant    traces    of 

27 

albumen. 
Do. 

28 

2 

400 

No  vomiting;  urine  greenish;  acid;  no  albumen. 

29 

Do. 

30 

395 

Do. 

May         1 

2 

Urine  normal;  dog  quite  well. 

Do. 

3 

395 

Do. 

Total.... 

4 

No.  2. 

1 1  gram  -=111  mg=7«  grains.) 


1902. 
Jan.       21 

23-24 

1 

9 

400 

L'"» 

2 

7.2 

5 

Before  experiment  dog  quite  normal;  urine  normal;  after  fir- 
ing dye  very  violent  vomiting  several  times. 
i  i  in.-  greenish  In  color;  add;  vary  mudb  albumen;  no  vomiting. 

Died  durta  i  the  ol 


COMPILED   DATA   UNDER    GREEN    TABLE    NUMBERS. 


117 


Experimental  data  by  Chlopin — Continued. 

No.  3. 

[1  gram=119  mg=83  grains.] 


Date.  Dose.       Weight 


24  hours' 
urine. 


General  condition  of  animal  and  urine. 


1902. 
Jan.       28 


30 
31 

Total... 


Grams. 


Kilos. 
8.4 


Before  experiment  dog  and  urine  normal;  soon  after  giving  dye 

vomiting  began,  lasting  over  an  hour;  dog  stands  wiih 

diificulty. 
During  ni^ht  dog  improved  somewhat,  began  to  eat;  drinks 

much;  soon  after  giving  dye  vomiting. 
During  night  vomiting  and  diarrhea;  during  night  30th,  31st, 

in  bad  condition;  does  not  take  food. 
During  night  31st  second  dog  found  dead  in  cage.    Cause  of 

death,  "  paralysis  of  the  heart." 


2.  Lewix  (Lehrbuch  der  Toxikologie,  1897,  p.  231):  In  the  case  of  one  workman,  in 
contrast  with  others  who  had  long  been  unaffected  by  this  substance,  itching, 
burning,  inflammation  and  swelling  of  hands  and  feet,  and  formation  of  blisters 
occurred. 

G.  T.  433. 

Trade  name. — Guinea  Green. 

Name  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Guinea  Green  B. 

Scientific  name. — Sodium  salt  of  diethyldibenzyl-diamido-tri- 
phenyl-carbinol-disulphonic  acid. 

Discovered. — 1883. 

Shade. — Green.     Offered  by  1  out  of  12  sources. 


FAVORABLE. 

1.  Chlopin  (p.  174):  On  his  own  experiments  classified  it  a* 
experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 
[1  gram=200  mg=  140  grains.] 


nonpoisonous. 


The 


Date. 

Dose. 

Weight 

24  hours' 
urine. 

1901. 
May   18 
19 

Grams. 
2 

Kilos. 
5 

cc. 
2.r»0 
2 16 

270 
270 
280 

20 

21 

a 

2 

2 

si 

10 

General  condition  of  animal  and  mine. 


Dog  and  urine  normal  before  experiment 

aton,  no  albumen;  vomited  el  night. 
No  vomiting. 

Urine  slightly  greenish;  no  albumen. 
Urine  normal  In  color  and  composition. 

Do. 

Da 

Do. 

I)... 
Do. 

Do, 
Da 


G.  T.  434. 
Track  names.—  Light  Greeo  SF  bluish;  Acid  Green. 
Scientific    name.     Sodium    Ball    of    dimethyldibenxyl-diainido-tri" 
phenyl-carbinol-1  risulphonic  acid. 


118 


COAL-TAR    COLORS   USED   HSf    FOOD  PRODUCTS. 


Discovered. — 1879. 

Shade. — Green.     Offered  by  1  out  of  12  sources. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Chlopin  (pp.  176-7):  Examined  this  color,  and  on  his  own  experiments  classes 
it  as  "nonpoisonous,  but  not  entirely  indifferent."  The  experimental  data 
are  as  follows : 

Experimental  data  by  Chlopin. 

No.  1. 

[1  gram=133  mg=93  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1902. 
Apr.   24 
25 

Grams. 
2 

Kilos. 
7.5 

cc. 
380 

Dog  and  urine  normal. 

Urine  green;  acid;  no  albumen. 

26 

347 
297 

Urine  green;  traces  of  albumen. 

27 

Do. 

28 

2 

Do. 

29 

Urine  green;  no  albumen. 

30 

360 

Urine  less  green;  no  albumen. 

31 

Do. 

May  1-3 

Do. 

370 

Do. 

Total  . 

4 

No.  2. 
[1  gram=110  mg=77  grains.] 


1902. 
Aug.    5 
6 

3 

9.1 

300 
310 

Dog  and  urine  normal. 

Urine  greenish,  acid,  no  albumen. 

7 

3 
3 
3 
3 

Do. 

8 

320 
350 

Do. 

9 

Do. 

10 

Do. 

11 

400 

350 

Do. 

12 

9 

Do. 

Total  . 

15 

DOUBTFUL. 

1.  Winogradow  (Zts.  Ndhr.  Genussm.  1903,  v.  6,  p.  689)  says  it  noticeably  retards 
digestive  action;  is  not  indifferent 

G.  T.  435. 

Trade  names. — Light  Green  SF  yellowish;  Acid  Green;  Acid  Green 
extra  cone. 

Names  under  which  it  was  offered  on  th<  United  Shifts  market  as  a 
food  color  in  1907. —  A.cid  Green  cone.  V  X;  Light  Green  SF  yellow 
shade;  Acid  Green  cone.  780 ;  Pistachio. 


COMPILED  DATA  UNDER   GREEN   TABLE   NUMBERS.  119 

Scientific    name. — Sodium    salt    of    diethyldibenzyl-diamido-tri- 
phenyl-carbinol-trisulphonic  acid. 
Discovered. — 1879. 
Shade. — Green.     Offered  by  4  out  of  12  sources. 

FAVORABLE. 

1.  Lieber  (p.  144):  The  animal  was  a  fully  developed  male  guinea  pig,  and  received 
per  kilogram  body  weight  240  milligrams,  or  108  grains  per  100  pounds,  live 
times  in  all,  every  other  day.  There  was  apparently  nothing  irregular  or  ab- 
normal observed  during  the  whole  test  of  nine  days. 

G.  T.  448. 

Tradenames. — Magenta;  Fuchsin;  Rosein;  Anilin  Red. 

Obsolete  names. — Rubin ;  Solf erino ;  Fuchsiacin ;  Rubianite ;  Azalein ; 
Erythrobenzin ;  Harmalin. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Magenta  powder  A;  Fuchsin  Crystals;  Magenta 
FABSRed  101. 

Scientific  name. — Mixture  of  hydrochlorid  or  acetate  of  pararo- 
sanilin  (triamidotriphenylcarbinol)  and  rosanilin  (triamidodiplienyl- 
tolylcarbinol) . 

Shade. — Bluish-red.     Offered  by  4  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Weyl  (p.  22):  "The  colors  examined     *    *    *     Fuchsin  were  (was)  found  to  be 

nonpoisonous-;"  "Similarly  a  hen  which  had  eaten  for  three  weeks  oate  covered 
with  fuchsin  was  in  good  health."     (p.  24.) 

3.  "According  to  Grandhomme  rabbits  bear  without  injury  fuchsin  free  from  arsenic 

*    *    *."     (p.  31.) 

4.  "Fuchsin    *    *    *    (is)  as  is  now  established,  almost  without  poisonous  action." 

(j>.  55.) 

5.  Fkaenkel  (p.  574),  quoting  Penzoldl.  says  that  it  Lb  entirely  nonpoisonous,  and 

completely  prevents  putrefaction. 
<;.  Permitted  by  the  law  of  Austria. 

7.  Lkwin  {Lehrbuch  dar  Toxtkologie,  189  0),  says  when  free  from  arsenic  it  is 

harmless. 

8.  Clouet  am.  Bbrgeron  (./.  pharm.  chim.,  I871t  i .  I  me  of  them  took 

•ually  500  milligrams,  that  i-.  7.7  grains  in  L6  days;  there  was  no  digestive 
disturbance  of  any  kind,  and  the  urine,  which  was  examined  daily,  contained 
no  albumen.  They  cite  a  case  of  Blight's  disease,  in  which  the  amount  of 
albumen  decreased  when  fuchsia  was  administered,  and  they  conclude  that 
fuchsin  may  be  good  Corsui  no  Blight's  disea 

(  KFAVOBABl  I  , 

1.  Forbidden  by  the  law  of  Fran  ,  p.  81.) 

2    Chlopim  (]  in  lined  this  color,  and  on  hi-  own  experiments  classes  it  as 

"Sn  acauee  "i"  vomiting  and  tracee  of  albumen."    'The  experimental 

data  are  ;i~  foU 


120  COAL-TAR   COLORS   USED   IX   FOOD   PRODUCTS. 

Experimental  data  by  Chlopin. 


Date. 

Dose.       Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Apr.   18 

Grams. 
3 

Kilos. 

cc. 
270 

280 

Dog  before  experiment  well  and  urine  normal;  vomited  several 

19 

times  after  receiving  dye. 
Urine  quite  red;  acid;  no  albumen;  general  condition  normal. 

20 

Do. 

21 

2 

320 

22 

Urine  darkish;  acid;  traces  albumen. 

23 

Color  normal;  no  albumen. 

24 

Do. 

Total. 

0 

Note.— This  sample  may  have  contained  some  phosphin,  G.  T.  532,  see  page  133. 

DOUBTFUL. 

1.  Wixogradow  (Zts.  Nahr.  Genussm.  1903,  v.  6,  p.  589)  says  it  almost  completely 
inhibits  digestion. 

G.  T.  450. 

Trade  names. — Hofmann  Violet;  Dahlia;  Red  Violet  5R  extra; 
Violet  R;  Iodin  Violet;  Primula;  Violet  5  R;  Violet  R  R. 

Scientific  name. — Mixture  of  the  hydrochlorids  or  acetates  of  the 
monodi-  or  trimethyl-  (or  ethyl-)  rosanilins  and  pararosanilins. 

Discovered. — 1863. 

Shade. — Violet.     Not  offered. 


FAVORABLE. 


1.  W'EYh(p.H):  "*    *    *    Anilin  Violet  (Dahlia) 

2.  Buss  lists  it  as  nonpoisonous. 


*     ■*     •* 


(is)  also  nonpoisonous. '  * 


IM  AVOUABLE. 


1.  Fraenkel  (p.  574)  quotes  Penzoldt,  and  says  it  completely  arrests  development, 
and  causes  muscular  paralysis. 

G.  T.  451. 

Trade  names. — Methyl  Violet  B;  Direct  Violet;  Dahlia;  Paris 
Violet;  Violet  de  Methylanilin ;  Pyoctanin. 

Names  under  which  it  was  offered  on  the  United,  States  market  as  a 
food  color  in  1907.— Methyl  Violet;  Methyl  Violc!  B;  Methyl  Violet 
BB  extra;  Methyl  Violet  3  BD. 

Scientific  name. — Hydrochloric!  of  penta-  and  bexamethyl-  para- 
rosanilin. 

Discovered. — 186 1 . 

Shade. — Violet.     Offered  by  5  out  of  L2  sources. 


I \\ ORABLB. 


1.  Permitted  by  Confectioners'  List. 

2.  Permitted  i>y  the  Austrian  law. 


COMPILED   DATA   UNDER   GREEX    TABLE    NUMBERS.  121 

3.  Weyl    (p.    24):    "  *    *    *    Anilin    Violet    (Dahlia)     *    *    *     [is]    also    non- 

poisonous." 

4.  "  *    *    *    Methyl  Violet  [is]  as  is  now  established,  without  poisonous  action. " 

(p.  5S). 

5.  Fraexkel  (p.  573):  "Methyl  Violet    *    *    *    is  relatively  n  on  poisonous." 

6.  Buss  lists  it  as  nonpoisonous. 

UNFAVORABLE. 

1.  Graefe  and  Braunschweig  (Fortschr.  Medizin,  1890,  i.  8t  p.  405):  "It  seems 

to  be  proven  that  damage  will  actually  result  even  in  the  case  of  most  cautious 
use,  which  we  are  sure  we  exercised." 

2.  Santori  (MokschotVs   Untersuchungen,  1895,   v.  15,  p.  52):  I.  A   dog  weighing 

7,600  grams  received  5.6  grams  dye  in  12  days;  this  amounts  to  61  milligrams 
per  kilo  per  day,  or  43  grains  per  100  pounds  per  day.  Continued  vomiting 
beginning  with  0.1  gram  dye;  progressive  emaciation  and  general  falling  away; 
catarrh  of  eyes  and  nose;  distinct  dislike  for  food  and  great  desire  to  sleep; 
temperature  below  normal,  urine  unchanged.  Loss  of  weight  1.000  grams,  or 
21  per  cent.  The  animal  died  on  the  thirteenth  day.  The  autopsy  showed  a 
pale  and  blood-poor  liver;  the  kidneys  were  in  a  typically  congested  condition 
and  contained  accumulations  of  blood  corpuscles.  II.  A  second  dog  weighing 
6,000  grams  received  3.8  grams  dye  in  14  days,  which  amounts  to  71.4  milli- 
grams per  kilo  per  day,  or  50  grains  per  100  pounds  per  day.  The  animal  died 
on  the  fourteenth  day.  There  was  daily  vomiting  and  rapid  emaciation;  final 
weight  loss  was  1,100  grams,  or  18.3  per  cent;  temperature  normal;  bloody 
urine  beginning  the  eighth  day.  The  autopsy  showed  a  blood-poor  liver,  soft 
and  swollen  epithelia;  kidneys  the  same  as  in  the  case  of  the  preceding  dog. 

G.  T.  457. 

Trade  names.— Anilin  Blue,  spirit-soluble;  Spirit  Blue;  Fine  Blue; 
Bleu  Lumiere ;  Opal  Blue;  Gentian  Blue  6B;  Hessian  Blue;  Bleu-de- 
Nuit. 

Scientific  name. — Hydrochloric!  sulphate  or  acetate  of  triphcnvlro- 
sanilin  and  triphcnylparaiosanilin. 

Discovered. — 1860-1862. 

Shade. — Greenish  blue;  not  offered. 

1  AVORAIJI.K. 

1.  Permitted  by  Confectioners'  List. 

LNTOR]       \foU9ChoU*i    ( '  nU  rtUckli  mjt  n ,    IS'.).',,    r.    15,    /'.  it     is   har: 

A  dog  wei  In:  ••<!  17  grams  dye  in  30  days,  which  amounts  to 

L26  milligrams  per  kilo  pet  <la>  or  B8  grains  per  LOO  pounds  per  day.  Weight 
remained  the  same,  genera]  condition  good,  urine  and  temperature  unchanged; 
killed  by  chloroform;  autopsy  showed  everything  normal. 

3.  Lbbbb  (p.  / 1  .  where  it  u  stated  to  be  permitted  by  the  Austrian  law  i  pp.  jj-j.;  , 

where  it  i-  stated  to  !>»•  permitted  by  the  Italian  law  {p.  31  ,  where  it  is  stated 
to  be  permitted  by  the  French  law  in  candies,  pastilles,  sweetmeats,  sauces, 

fruit-,  ami  certain  liqueur-  ordinarily  not  colored. 

4.  Wiyi.  </>.  ..'.'),  quoting  Sonnenkalb  (p.  t4),  quoting  Grandhomme. 

iaj  \k!  1. 1 (p.  I  that  it  it  effective  in  only  5  percent  of  malaria  cases. 

6.  Permitted  by  the  law  of  Austria. 

7.  l'.i  si  lists  it  as  ii  mpoi  onous. 


122 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


UNFAVORABLE. 

1.  Weyl  (p.  23),  quoting  Friedrich,  where  poisoning  was  produced  in  a  young  man 
engaged  in  packing  this  dye. 

G.  T.  459. 

Trade  names. — Iodin  Green;  Pomona  Green;  Night  Green;  Vert 
Lumiere. 

Scientific  name. — Zinc-double-chlorid  of  heptamethyl-rosanilin- 
chlorid. 

Discovered  and  patented. — 1866. 

Shade. — Green.     Not  offered. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Chlopin  (p.  175)  on  his  own  experiments  classes  it  as  "suspicious."     (See  p.  181). 
The  experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 
[1  gram=lG7  mg=117  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
May     9 
10 

Grams. 
G 

Kilos. 
G 

cc. 
420 
470 
441 
420 
390 
400 
442 
370 

Before  experiment  dog  and  urine  normal. 
Do. 

11 

Ufine  slightly  greenish;  no  albumen. 
Do. 

12 

2 

13 

Urine  has  greenish  opalescence;  traces  of  albumen. 

14 

Do. 

15 

Urine  has  greenish  opalescence;  no  albumen. 
Do. 

16 

2 

17 

Urine  has  greenish  opalescence;  traces  of  albumen. 

18 

400 

Normal  color;  no  albumen. 

Total.. 

G 

2.   Buss  lists  it  as  poisonous. 


DOIJHTFUL. 


1.  Winogradow  (ZtS.  NcJir.  Gcnussm.,  1903,  V.  6,  p.  689)  says  it   noticeably  retards 
digestive  action;  is  not  indifferent. 

G.  T.  462. 


Trade  names. — Acid  Magenta;  Acid  Fuchsin;  Acid  Rubin;  Fuch- 
sin  S;  Acid  Rosein ;  Rubin  S. 

Names  under  which  it  was  offered  on  (he  United  States  market  as  a 
food  color  in  t907.-   Acid  Magenta  Powdered;  Acid  Magenta. 

Scientific  name. — Mixture  of  the  sodium  or  ammonium  salts  of  the 
trisulphonic  acids  of  rosanilin  and  pararosanilin, 

Discovered.     L877. 

Shade.     Red.    Offered  by  2  out  of  12  sources. 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 


123 


FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Cazeneuve  (Arch.  gen.  mid.,  1886,  p.  753)  says  it  may  be  taken  without  effect  by 

man  and  animals,  sick  or  well,  in  large  doses. 

3.  Weyl  (p.  55),  where  he  says  that  it  is  established  of  this  color  that  it  is  almost  with- 

out poisonous  action. 
2.  Lieber  (p.  14),  where  it  is  stated  to  be  permitted  by  the  law  of  Austria  (p.  31), 
where  it  is  stated  to  be  permitted  by  the  law  of  France  for  confectionery,  cor- 
dials, and  the  like. 

5.  Permitted  by  the  law  of  Austria. 

6.  Permitted  by  the  law  of  Italy. 

7.  Cazeneuve  and  Lefine  (Compt.  rend.,  1885,  v.  101,  p.  1011):     A.  Dog:  15  kilos 

weight,  received — 


Days. 

Grains. 

Milligrams 
per  kilo. 

Grains  per 

100  pounds. 

15 
5 
5 
5 

1 
2 
5 
10 

67 

134 
335 
G70 

47 

94 

235 

470 

No  diarrhea;  no  vomiting;  no  albuminuria;  urine  colored  only  occasionally, 
but  did  contain  the  leuco  compound  of  the  dye.  B.  Man:  1.  Afflicted  with 
Bright's  disease;  took  two  grams  daily  for  one  week;  no  effect.  2.  Afflicted 
with  renal  cirrhosis;  four  grams  daily  for  several  days;  no  effect.  3.  A  well 
man  took  four  grams  daily  for  several  days;  no  effect. 
8.  Cazeneuve  and  Lefine  (Bull,  de  Vacad.  de  mid.  1886,  p.  643):  Tolerated  by  man, 
sick  or  well. 

G.  T.  467. 

Trade  name. — Acid  Violet  6B. 

Scientific  name. — Sodium  salt  of  dimethyl  diethyl  dihenzyl  triamido 

tri phenyl  carbinol  disulphonic  acid. 
Discovered  and  patented. — 1889. 
Shade. — Violet.     Not  offered. 

FAVORABLE. 

1.  Santori  (MoleschotCs  Untersuchungen,  1895,  r.  15,  p.  54)'.  A  dog  weighing  4,260 
grama  received  12.5  grama  dye  in  28  days,  which  amounts  to  LOB  milligrams  per 

kilo  per  day,  or  74  grains  per  100  pounds  per  day.     The  dog  vomited  the  Color 

only  two  or  three  times  and  was  otherwise  normal.  Appetite,  temperature, 
and  urine  all  remained  normal.  Conclusion:  Nonpoisonous;  autopsy  also 
showed  everything  normal. 


Nothing. 


[JNPAVORABL] 


G.  T.  477. 


Tradi  names.-— Alkali  Blue;  Nicholson  Blue;  Past  Blue. 
Scientific  /num.  -Mixture  of  Bodiuxn  aaltfl  of  triphenyl  rosanilin 
monoeulphonic  acid  and  of  triphenyl  para  roBanilin-monosulphonio 

acid. 


124 


COAL-TAE  COLORS  USED  IN  FOOD  PRODUCTS. 


Discovered  and  patented. — 1862. 
Shade. — Blue.     Xot  offered. 

FAVORABLE. 

1.  Santori  (MoleschotVs  Untersuchungen,  1895,  i\  15,  p.  45):  A  dog  weighing  4,500 
grams  received  25  grams  dye  in  30  days,  which  amounts  to  185  milligrams  per 
kilo  per  day,  or  129.5  grains  per  100  pounds  per  day.  The  urine  remained  of 
normal  color,  but  the  stool  was  a  deep  blue  black.  Throughout  the  whole  time 
the  animal  was  in  perfect  health.  Killed  with  chloroform;  autopsy  showed 
everything  normal. 

UNFAVORABLE. 

Nothing. 

G.  T.  478. 

Trade  names. — Bavarian  Blue  DSF;  Methyl  Blue,  water-soluble; 
Navy  Blue  B;  Methyl  Blue  for  silk  MLB. 

Scientific  name. — Sodium  salt  of  triphenyl  pararosanilin  di-  and 
tri-sulpho  acid. 

Discovered. — 1862;  not  patented. 

Shade. — Blue.     Not  offered. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Chlopin  (p.  170)  examined  this  color,  and  on  his  own  experiments  classed  it 
"nonpoisonous  but  not  quite  indifferent." 

Experimental  data  by  Chlopin. 
[1  gram=115mg=Sl  grains.] 


Date.        Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
May    18 
19 

Grams. 
2 

Kilos. 
8.7 

450  |  Dog  and .urine  quite  normal. 

23 

380 
370 

Do. 

24 

2 

Do. 

25 

Do. 

2 

Do. 

27 

370 
320 

Do. 

28 

2 

Do. 

2'J 

Do. 

30 

2 

Urine  slightly  greenish;  traces  of  albumen:  acid. 

Do. 

31 

June     1 

Do. 

2 

327 

Do. 

3 

Do. 

4 

3 

Do. 

:. 

[Trine  slightly  greenish;  traoas  of  albumen;  acid;  diarrhea. 

t. 

3 

105 

Do. 

7 

i  rine  slightly  greenish;  traces  of  albumen;  add. 

s 

3 

M6 
868 

870 

Da 

<J 

Do. 

10 

3 

Do. 

11    1.', 

Lfl 

Do. 

H.5 

Do. 

22 

•  Dally. 


COMPILED   DATA   UNDER    GREEX    TABLE    NUMBERS. 


125 


G.  T.  479. 

Trade  names. — Methyl  Blue  O;  Brilliant  Cotton  Blue  greenish; 
XL  Soluble  Blue;  Diphenylamin  Blue;  Bavarian  Blue  DBF;  Soluble 
Blue  8B  and  10B;  Helvetia  Blue. 

Scientific  name. — Sodium  salt  of  triphenyl-pararosanilin  tri- 
sulphonic  acid. 

Discovered  and  patented. — 1862. 

Shade. — Blue.     Not  offered. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Chlopin  (p.  168)  examined  this  color  and  on  his  own  experiments  classed  it 
"suspicious"  or  "nonsuspicious"  dependent  upon  the  make  of  goods. 

Experimental  data  by  Chlopin. 

No.  l. 

[1  gram=75  mg=52  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
May   14 
15 

Grams.        Kilos. 
2             13.4 

cc. 
460 

Dog  normal;  no  albumen. 

Color  chocolate-brown;  insignificant  traces  of  albumen. 

16 
17 

Total.. 

2 

Color  same;  no  albumen. 



410 

Urine  normal;  no  albumen;  dog  is  well. 

4 

No.  2. 
[1  gram  =  152  mg.  =  lot;  grains.] 


1901. 
Nov.  12 
13 

3 

6.6 

300 

15 

3 
3 
3 
3 

16 

360 
305 
330 

17 

19 

20 

21 

22 

6.8 

Total.. 

15 

Dog  quite  well;  urine  normal  color;  acid;  no  albumen. 

Do. 

Do. 

Do. 
Urine  scarcely  perceptible  greenish  sheen;  acid;  no  albumen. 
I  line  greenish  color;  no  albumen. 

i  rine  darker;  no  albumen. 
Urine  color  normal;  no  albumen. 
Color  almost  normal. 


This  preparation  from  Moscow;  ooi  suspicious. 

No.  3  (Mi:iu  K's   ri:i.i\vK\ii"N 
[l  gram •=  147  nag    103 grains.] 


Date. 

Weight. 

M  boms' 
mine. 

Genera]  condition  of  animal  and  mine. 

Feb,  is 

19 

3 

;t 

MO 

klbumen; 

•Mai  yellow  ("lot .  _'  hours  after  giving  dye  vomit] 
Vomiting  stopped;  diarrhea;  urine  chooolate-brown;   i 
lerable  albumen;  appetite  nol  • 

During  night  diarrhea;  no  \omiting;  urine  brown;  a.  id.  trai  e-    f 
albumen;  without  acid  urine  becomes  blue. 

ii  he  a;  no  vomiting;  urine  bron  a;  tracei  of  albumen. 

n 

■21 

n 

i  rlne  brae  chocolate-brown;  otherwise  non                  toquired 

u   nil                            liter. 

15 

Conclusion:   "8u«pi  i 


126        COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

G.  T.  480. 

Trade  names. — Soluble  Blue;  China  Blue;  Cotton  Blue;  Bleu 
Marine;  Water  Blue;  Water  Blue  6  B  extra;  London  Blue  extra. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Pure  Soluble  Blue. 

Scientific  name. — Sodium,  ammonium  or  calcium  salt  of  the  tri- 
sulphonic  acid  (with  some  disulphonic  acid)  of  triphenyl-rosanilin  and 
triphenyl-pararosanilin. 

Discovered  and  patented. — 1862. 

Shade. — Blue.     Offered  by  1  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  law  of  Austria. 

2.  Lieber  (p.  147):  A  guinea  pig  received  306  milligrams  per  kilogram  body  weight, 

or  214  grains  per  100  pounds,  once  a  day  seven  times  every  other  day;  the  weight 
remained  substantially  constant,  a  slight  gain  of  less  than  |  per  cent  being  noted. 
"Nothing  irregular  or  disturbing  whatsoever  was  observed  during  the  whole 
period." 

3.  Santori  (Moleschott's  Untersuchungen,  1895,  v.  15,  p.  45):  A  dog  weighing  4,500 

grams  received  30  grams  dye  in  30  days  which  amounts  to  223  milligrams  per 
kilo  per  day  or  156  grains  per  100  pounds  per  day.  Animal  remained  well 
throughout;  no  loss  of  weight  or  appetite;  urine  normal  color,  stool  deep  blue; 
killed  with  chloroform;  autopsy  showed  a  pea-green  coloring  of  the  cortex  of 
the  kidneys. 

UNFAVORABLE. 

1.  Fraenkel  (p.  574),  quoting  Penzoldt,  says  that  it  completely  arrests  germ  devel- 

opment, and  causes  changes  internally. 

2.  Saxtoki  (Moleschott's  Untersuchungen,  1895,  v.  15,  p.  46):  Regards  this  as  injurious 

hypodermically,  but  not  through  mouth.  A  dog  weighing  4,000  grams  received 
3.5  grams  of  dye  hypodermically  in  16  days,  at  the  end  of  which  time  he  died; 
this  amounts  to  55  milligrams  per  kilo  per  day  or  38.5  grains  per  100  pounds 
per  day.  The  autopsy  showed  the  liver  to  be  free  from  blood;  kidneys  soft, 
and  congested;  all  organs  swollen  and  colored. 

G.  T.  483. 

Trade  names. — Aurin;  Rosolic  Acid;  Yellow  Corallin. 
Scientific  name. — Mixture  of  aurin  (trioxytriphenvl-caibinol)  oxi- 
dized aurin,  metli  vlauiin,  and  pseudo-rosolic  acid  (corallin  phthalin). 
Discovered. — 18.']  4. 
Shade, — Yellowish  brown.     Not  offered. 

i  \  \  ORABLB. 

].  I.i.win-  [Lehrbuch  </>/■  Toxikologie,  1897,  p.    151  :  RosolicAcid  Is  positively  nan- 
poisonous. 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 


127 


UNFAVORABLE. 


1.  Chlopin  (p.  167)  examined  this  color,  and  on  his  own  experiments  classes  it  as 
"strongly  poisonous."    The  experimental  data  are  as  follows: 

[1  gram=137  mg=96  grains.] 


Date. 

Dose. 

w^hja* 

General  condition  of  animal  and  urine. 

1902. 
Mar.   12 

13 

Grams. 

1 

2 
3 
3 

Kilos. 
7.3 

cc. 
330 

375 
300 

Before  experiment  dog  quite  well;  urine  normal  color;  acid;  no 

albumen. 
Diarrhea;  urine  faint  red. 

14 

Diarrhea;  lassitude:  eats  little;  urine  red;  no  albumen. 

15 

Violent  diarrhea  and  vomiting;  dog  stands  on  feet  with  diffi- 
culty; eats  nothing. 

Same  conditions  as  on  preceding  day;  dog  sick  for  a  long  time 
after. 

16 

Total.. 

9 

2.  Prohibited  by  the  German  law  of  1887. 

3.  Prohibited  by  the  Belgian  law  of  June  17,  1891. 

4.  Buss  lists  it  as  poisonous. 

DOUBTFUL. 

1.  Lewin  (Lehrbuch  der  Toj Otologic,  1897,  p.  231):  Rosolic  Acid  is  positively  non- 
poisonous.  Small  animals  can  take  1  gram  and  more  of  it.  In  Austria  it  is 
prohibited  for  use  in  coloring  foods.  Corallins,  or  red  (Pa?onin)  or  yellow 
colors,  consisting  of  Aurin  and  Rosolic  Acid  were  regarded  as  poisonous 
because  in  experiments  on  man  and  animals  illness  occurred,  but  are  said  to 
be  poisonous  only  in  the  presence  of  arsenic,  phenol,  or  anilin.  These  sub 
stances  are  prohibited  in  the  coloring  of  food. 

G.  T.  488  or  490. 

Trade  name. — Victoria  Blue;  Victoria  Blue  B;  Victoria  Blue  4R. 
Scientific  names. — Hydrochloric!   of   phenyltetra   (penta)   uiethvl- 
triamido-diphenyl-al])lia-naj)htliyl-carbinol  (note:  4K  is  bracketed). 
Discovered  and  patented. — 1883. 
Shade. — Blue.     Not  offered. 


Nothing. 


I A\ uUAHLE. 


UNFAVOlIAHl  .!•: 


chott'i  Untersuchungen,  1895,  v.  i~>,  p.  47)\  A  dog  weighing 
gran  una  dye  in  22  days,  which  amounts  to  45  milligram! 

per  kilo  per  day  or  32  grains  per  100  pounds  per  day.    Alter  receiving  L.5 
grama  the  annual  Buffered  copious  continuous  Balivation,  anemia,  and  emacia- 
tion and  occasional  vomiting.    The  urine's  color  did  not  change;  th- 
ine blue;  temperature  slightly  above  and  below  aormal;  although  highly 
emaciated  (loss  in  weight  wi  imsorSS]  per  cent)  the  animal  retained 

fa  appetite;  animal  died  on  the  morning  of  the  23d  day.    The  autopsy  showed 
phagus,  stomach,  and  intestines  colored  deep  blue  and  filled  with  ■  green- 
ish scum,  extended  and  strong  catarrh  of  the  stomach  and  intestines;  kidneys 
and  liver  contained  very  little  blood.    Conclusion:  Poison 

1 1  :  It  is  uncertain  which  of  these  two  dyes  Santori  used 


128 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

G.  T.  502. 


Trade  name. — Rhodamin  G  and  G  extra. 
Scientific  name. — Chiefly  Triethylrhodamin. 
Discovered  and  patented. — 1891. 
Shade. — Bluish.     Offered  by  2  out  of  12  sources. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Chlopin  (p.  184)  examined  this  color,  and  on  his  own  experiments  classes  it  as 
"suspicious."     The  experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 
fl  gram=  167  mg=  117  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1903. 
Feb.  18 

19 

Grams. 
3 

3 

Kilos. 
6 

cc. 
310 

Dog  normal;  urine  acid;  no  albumen;  after  2  hours  thin  stool; 

remainder  of  day  lively;  good  appetite. 
Urine  fuchsin  color,  acid,  no  albumen;  stool  and  appetite  normal. 

20 

3 
3 

3 

Goes  to  stool  without  results;  otherwise  as  above. 

21 

270 
320 

Do. 

22 

Do. 

23 



Goes  to  stool  without  results;  urine  normal  after  8  days. 

Total.. 

15 

G.  T.  504. 

Trade  names. — Rhodamin  B;  Rhodamin  O;  Safranilin. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Rhodamin  B  extra;  Rhodamin;  Rhodamin  B. 

Scientific  name. — Hydrochlorid  of  diethylmeta-amido-phenol- 
phthalein. 

Discovered  and  patented. — 1887. 

Shade. — Bluish  red.     Offered  by  5  out  of  12  sources. 

FAVORABLE. 

1.  Lieber  (p.  141):  A  young  female  rabbit  received  339  milligram  body  weight,  or 
237  grains  per  100  pounds,  five  limes  on  alternate  days.  "During  the  whole 
period  the  animal  seemed  to  be  perfectly  at  ease,  was  lively,  displayed  good 
appetite,  and  gained  steadily  *  *  *  •"  The  gain  in  weight  was,  roughly, 
7  per  cent. 

i   \  I  \\  i»l;.\  Hi  l  . 

l .  <  Ihlokm  (pp.  U  axnined  this  color,  and  on  bis  o*  d  experiments  classifies 

it  M  "not  poisonous,  but  not  entirely  indifferent;  suspicious."     The  experi- 
mental data  are  as  follow  -: 


COMPILED   DATA    UNDER   GREEX    TABLE    NUMBERS. 

Experimental  data  by  Chlopin. 
f  1  gram  =  109  mg  =  76  grains.] 


129 


Date. 

Dose. 

Weight,  j"*™* 

General  condition  of  animal  and  urine. 

1904. 
Feb.   18 

19 

Grams. 
3 

3 

3 

3 
3 

Kilo*. 
9.2 

cc. 
420 

400 

400 

Dog  normal;  urine  aci<l,  no  albumen;  strong  yellow  color;"? 
hours  after  giving  color  tiiin  stool. 

Urine  colored  wine  red,  strong  fluorescence,  disappears  on  boil- 
ing, and  reappears  on  cooling;  no  albumen. 

Thin  stool;  no  change  in  other  resp 

No  diarrhea;  no  change  in  other  respects. 

General  condition  goo<J;  urine  red  and  acid;  no  albumen. 

20 

21 

22 

420 

Total.. 

15 

Dog  recovers. 


G.  T.  512. 


Trade  names. — Eosin;  Eosin  A;  Eosin  B;  Eosin  A  extra;  Eosin 
Yellowish;  Eosin  G  G  F;  Water-soluble  Eosin;  Eosin  3  J  and  4  J 
extra. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Erythrosin  I  X;  Eosin  J;  Eosin  Y. 

Scientific  name. — Alkali  salts  of  Tetra-bromo-fluorescein. 

Discovered. — 1 S74 . 

Shade. — Yellowish  red.     Offered  by  3  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners1  List. 

2.  We  yl  ( p.  SI )'.  "According  to  Grandhomme,  rabbits  bear  without  injury    *    *    * 

Eosin    *    *    *•' 

3.  Permitted  by  the  law  of  Austria. 

4.  Buss  lists  it  as  di  opoisonous. 


UN  FAVORABLE. 


1.  Lewin  (Lfhrbuch  der  Toxikologie,  1897,  p.  tSl):  "The  continued  use  of    these 

coloring  matters,  as  well  asof  Phenolphthalein,  which  becomes  colored  in  the 
ird  as  harmful,  and,  in  tact,  through  action  as  coloring  matters." 

2.  Forbidden  by  the  Italian  law. 

G.  T.  516. 

Tradenames.  ErythrosinG;  PyrosinJ;  Jaune  d' Orient;  Dianihii 
( i :   [odeosic  ( r. 

Norm  under  which  it  was  offered  on  tin  United  States  market  as  a  food 
color  in  1907.     Erythrosii]  yellowish  shade. 

Scientific  tanu      Sodium  or  potassium  -alt  of  diiodofluoresceiiL 

'•1       Bull 


130 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Discovered . — 1875. 
Shade. — Yellowish  red 


Offered  bv  1  out  of  12  sources. 


Nothing. 


FAVORABLE. 


I"  \"  FAVORABLE. 


1.  Chlopin  (p.  181):  Examined  this  color,  and  on  his  own  experiments  reports  it  as 
"injurious  because  of  light  albuminuria,  vomiting,  and  diarrhea.''  The 
experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 

No.  I. 

[1  gram  =  156  mg  =  109  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  ami  urine. 

1901. 
Apr.   24 
25 

Grams. 
2 

Kilos. 
C.4 

cc. 
360 
353 
368 

370 

Before  experiment  dog  and  urine  normal. 
Urine  red  yellow  with  greenish  aheen;  add;  no  albumen. 
Urine  red  yellow  with  greenish  sheen;  acid;   trace  of  albumen. 
Do. 

26 



27 

28 

2 

Urine  red  yellow  with  greenish  sheen;  acid;  no  albumen. 
Do. 

29 

355 

365 
365 

30 

Do. 

May     3 

Do. 

Total . 

4 

No.  2. 

[1  gram  =  152  mg      106  grains.] 


1901. 
Noy.  24 

6.6 

345 

25 

3 

3 
3 
3 

3 

26 

27 

28 

3S0 
340 

29 

30 

Dec.  2-3 

Total . 

•  15 

Dot,'  and  urine  normal. 

Do. 
Urine  fluorescent  orange;  no  albumen. 
Vomiting,  diarrhea;  urine  orange;  no  albumen. 
No  vomiting  and  no  diarrhea;  urine  fluorescent, 
men. 

Do. 

Do. 
Color  and  coin  posit  ion  of  urine  normal;  dog 


d;  no  alba* 


DOFHTFCI 


i    WiNoatfADOw  (Zts.  Nahr.  Genussm.  t90S,  v.  6,  p.  589)  Bays  it  almost  completely 
inhibits  digestion. 

G.  T.  517. 


Trade  names, — Erythrosin;  Erythrosin  B;  Eodeosin  Bj  Eosln  J; 
Erythrosin  I);  Pyrosin  I>;  Eosin  Bluish. 

Names  under  which  it  woe  offered  on  tin  United  States  market  as  a 
food  color  in  t907. — Erythrosin  Yellow  Shade;  Erythrosin  B;  Ery- 
throsin. 


COMPILED    DATA    UN  DEB    GREEN    TABLE    NUMBERS.  131 

Scientific  name. — Sodium  or  potassium  salt  of  tetraiodofluoresceiru 

Discovered. — 1876. 

Shade. — Bluish  red.     Offered  by  5  out  of  12  sources. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

2.  Wetl  •  <>.  ■-.'      "  According  to  Grandhomme,  rabbits  bear  without  injury    *    *    * 

Erythrosine    *    *    *." 

3.  Permitted  by  the  laws  of  Prance 

4.  Permitted  by  the  law  of  Austria. 

5.  Fbaenkel  {p.  574)'-    "Rose  Bengal     *    *  produces  no  noticeable  disturb- 

ances." 

6.  Buss  lists  it  as  nonpoisonous. 

UNFAVORABLE. 

1.  Lewi\  (Lehrbuch  d?r   Toxikologic,  1897,  p.    131)'.  "The  continued    use  of   these 
coloring  matters,  as  well  as  of  phenolphthalein,  which  becomes  colored  in  the 

system,  I  regard  as  harmful,  and,  in  fact,  through  ad  ion  as  coloring  matters." 

G.  T.  520. 

Trade  names. — Rose  Bengal;  Rose  Bengal  A  T:  Rose  Bengal  X; 
Rose  Bengal  G. 

Names  under  which  it  was  offered  on  tfa  United  States  market  as  a 
food  color  in  1907. — Rose  Bengal  B;  Phloxin  B. 

Scientific  name. — Alkaline  salt  of  tetraiododichlorofluorescein. 

Discovered.    -1875. 

Shade. — Bluish  red.     Offered  by  2  out  of  12  sources. 

I AVORABLE. 

1.  Permitted  by  Confectioners5  List. 

G.  T.  521. 

Troth   names. — Phloxin:  Phloxin  TA ;  Kosin  10B. 

Scientific  name. — Sodium  Bait  of  tetrabromotetrachlorofluorescein. 

Disco;  red. — 1882. 

Shade.— Red.     \<>t  offered. 

kav«»i:\iii  I 

l    Pa  mitted  by  <  'onfectioners'  List. 

2.  Permitted  by  ili<-  Austrian  law. 

mined  this  color,  and  on  bis  own  experiment!  rliwiflra  ii  m 
"nonpoisonous. "    The  experimental  data  are  m  follows: 


132 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

Experimental  data  by  Chlopin. 

No.  l. 

[1  gram=  143  mg=  100  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
Apr.   10 

11 

Grams. 

1 

Kilos. 

7.0 

cc. 
380 
370 
370 
370 

Dog  and  urine  quite  normal. 
Do. 

12 

Do. 

13 

3 

Do. 

14 

Urine  orange. 

15 

390 

Do. 

Total.. 

4 

No.  2. 
[1  gram=116  mg=Sl  grains.] 


1901. 
Nov.    3 
4 

3 

8.G 

450 
430 

Dog  well;  urine  normal  color;  acid; 
Urine  orange;  no  albumeu. 

Do. 

Do. 

Do. 

Do. 

Do. 

Do. 
Color  almost  normal;  no  albumen. 

Do. 

no  albumen. 

5 

3 

6 

400 
440 
430 
450 
400 

7 

3 
3 

g 

9 

10 

3 

11 

12-14 

Total.. 

15 

G.  T.  527. 

Trade  names. — Coerulein  S;  Alizarin  Green;  Anthracene  Green. 
Scientific  name. — Sodium  bisulphite  compound  of  coerulein. 
Discovered. — 1879. 
Shade. — Black.     Not  offered. 

FAVORABLE. 

1.  Chlopin  (pp.  186-7)  examined  this  color,  and  on  his  own  experiments  reports  it  as 
"non poisonous,  and  not  sufficient  data  to  regard  it  as  suspicious."  The  exper- 
imental data  are  as  follows: 

Experimental  data  by  Chlopin. 

No.  l. 
[1  gram  ----- 117  mg—  lil.'i  grains.] 


Date. 

Dose. 

Weight. 

21  hours' 

urine. 

Qeaeral  condition  of  animal  and  urine. 

I'.HM. 

drum*. 
2 

Kiln,. 

ti.  S 

cc. 
820 
880 
800 
830 
800 

Before  experiment  dog  quite  normal. 
i  i  me  normal;  acid;  no  albumen. 

Sept    1 

2 

8 

8 

Do 

lnn«'  has  scarcely  perceptible  sheen;  m>  albumen. 

3 

Do. 

4 
6 

7 

8 
8 
8 
8 

Do. 

800 

Do. 

Do 

Nothing  abnormal. 

Do. 

10 

11 

2 

Do. 

Do. 

Do 

22 

COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 

Experimental  data  by  Chlopin — Continued. 

Xo.  2. 

11  gram=lG7  mg=117  grains.] 


133 


Date. 

Dose. 

Weight. 

2  uruiT8                         General  condition  of  animal  and  urine. 

1902. 
Mar.     3 
4 

Grams. 
2 
3 
3 

2 

Kilos. 
6 

cc. 
270 
250 
265 

Before  experiment  dog  quite  well;  urine  normal. 
Urine  vellow  with  orange  sheen:  acid;  no  albumen. 

5 

Thin  stool  twice;  urine  dark  yellow  with  greenish  sheen;  aci<l: 

no  albumen. 
Stool  normal;   urine  yellow  green;  acid;  no  albumen;  general 

condition  quite  well! 

6 

Total.. 

10 

DOUBTFUL. 

1.  Winogradow  (Zts.  Ndhr.  Genussm.,  1903,  v.  6\  p.  589)  says  it  almost  completely 
inhibits  digestion. 

G.  T.  530. 

Trade  name. — Benzoflavin. 

Scientific  name. — Hydrochloric!  of  diamido-phenyl-dimethyl-acridin. 

Discovered. — 1887. 

Shade. — Brownish  orange  yellow.     Not  offered. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Chlopin  (p.  189)  on  his  own  experiments  regards  this  color  as  suspicious.    The 
experimental  data  are  as  follows: 

Experimental  data  by  Chlopin . 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1901. 
May     3 

4 

Grams. 
2 

Kilos. 

cc. 
365 
391 

Before  experiment  dog  well  and  urine  normal. 

Dog  ate  poorlv;  traces  of  albumen. 
Do. 

5 

2 

6 

330 
375 

Urine  greenish  sheen;  acid. 

7 

2 

Color  same;  no  albumen. 

8 

Do. 

0 

Do. 

Total.. 

6 

G.  T.  532. 

Tradt  names,  -Phoephin;  Xanthin;  Leather  Yellow;  Philadelphia 
Xello*  Q, 

Scientific  name, — Nitrate  of  chrysanilio  (unsym.  diamido-phenyl- 
acridin    and  homologues. 

Discovered.     1862. 

Shade, — Orange  yellow.     X<>t  offered. 


I    <i\  iilHIII   K. 


Nothing. 


134 


COAL-TAR    COLORS    rsi.])    IN    FOOD    PRODUCTS. 


UNFAVORABLE. 

1 .  Chlopin  I  p.  190  I  reports  Fuchsia  containing  Phoephin  as  suspicious. 

2.  On  his  own  experiments  aaya  this  color  •"docs  not  belong  to  the  poisonous  colors, 

but  is  not  wholly  harmless.  "     The  experimental  data  arc  as  follows: 

Experimental  data  by  Chlopin. 
[l  gram— 147  mg=103  grains.] 


! 

Date.         Dose        Weight. 

urine18                        General  condition  of  animal  and  urine. 

1901.     ;    Grams. 
Apr.    15    

Kilos. 
6.8 

cc. 
390 

350 
350 

]>ok  well;  urine  normal. 
Do. 

16                  2 

17    

Do. 

18                   3 

Urine  yellower  than  normal;  vomited  several  limes  after  taking 

dye;  no  albumen. 
Urine  same;  no  vomiting. 

19    

330 
370 

21                    2 

22    

No  vomiting;  urine  same. 
Color  normal. 

23 ; 

24     

Dog  well;  urine  normal. 

Total . .                7 

3.  (p.  178):  See  experimental  data  on  G.  T.  448,  which  also  applies  to  this  color. 

4.  Fraenkel  (p.  578):  Where  its  physiological  action  is  compared  with  quinin  its 

action  on  protozoa  is  far  greater.  "The  Phosphins  are  locally  strong  irritants, 
and  producers  of  inflammation  of  medium  poisonous  nature  so  that  humans 
can  very  well  bear  400  milligrams,  or  6.17  grains. 

5.  Lewin  (Lehrbuch  der   Toxikologic,  1897,  p.  232):   "Phosphin     *    *    *    produces 

in  humans,  in  doses  up  to  1  gram,  vomiting  and  diarrhea." 


DOUBTFUL. 


WlNOGRADOW   (ZtS.    Xahr.   Crnimm. 

inhibits  digestion. 


l'jo.).  v.  6*,  p.  589)  says  it  almost  completely 


G.  T.  563. 

Trade  names. — Alizarin  Blue  S;  Anthracene  Blue  S;  Alizarin 
Blue  ABS. 

Scientific  name. — Sodium  bisulphite  compound  of  dioxyanthra- 
quinonc-beta-quinolin. 

Discovered  and  patented. — 1 88 1 . 

SJoade. — Blue,     Not  offered. 


I     Permitted  bv  law  of  Austria. 


FA  VOKABLK. 


i    \l   \  \  ORABLE. 


<  Ihlopin   p.  171):  ( m  authority  no1  given  reports  this  color  as  poisonous  or  harmful. 

Ehrlich  (Da*  SauentoffbeduerfniM  des  Organismus,  1885,  p.  M):  "Per  kilogram 

of  rabbit,  12- 1 5  CC  of  this  solution   in  general    produce  death   within   the  first 

quarter  of  an  hour;  whereat  i  cc  of  the  same  did  not  usually  produce  it,  and 
7  cc  represent  a  medium,  when  properly  applied,  fatal  dose."    (This  solution 

contained   DOi   to  exceed    17  per  cent,   coloring    matter;  each  cubic  centimeter 

represents  L70  milligrams  per  kilogram  body  weight,  or  L19  grains  per  100  pounds; 

the  coloring  matter  was  introduced  subcutaneously.) 

lists  it  as  poisonous. 


COMPILED    DATA    UNDER   GREEN    TABLE    NUMBERS.  135 

G.  T.  572. 

Tradename. — Indophenol  white;  Leucindophenol. 
Scientific  name. — Tin  compound  of  dhnethyl-para-amido-phenyl- 
para-oxy-alphanaphthylamin. 
Discovered. — 1881 . 
Shade. — Blue.     Xot  offered. 

FAVORABLE. 

Nothing. 

UNFAVORABLE. 

1.  Santori  {MoleschotVs  Untersuchungen,  1895,  v.  15,  p.  57):  A  dog  weighing  4,000 
grams  received  18  grams  dye  in  30  days,  which  amounts  to  150  milligrams  per  kilo 
per  day  or  105  grains  per  100  pounds  per  day.  Temperature,  urine,  and  weight 
all  remained  unchanged.  Animal  killed  with  chloroform;  autopsy  showed 
fatty  degeneration  of  the  liver;  everything  else  normal.  (Santori  classes  this 
color  as  "not  nonpoisonous.") 

G.  T.  574. 

Trade  names. — Ursol  D;  Ursol  P;  Ursol  DD. 

Scientific  name. — Hydrochlorids  of  para-phenylene  diamin,  para- 
amidophenol,  and  diamidodiphenylamin,  respectively. 
Discovered. — 1888. 
Shade. — Brown  to  black.     Not  offered. 

FAVORABLE. 

Nothing. 

UNFAVORABLE. 

1.  Chlopin  (p.  214)  examined  this  color,  and  on  his  own  experiments  reports  it  as 
"strongly  poisonous."  On  January  15,  1901,  a  dog  weighing  18.4  kilos  was 
given  3  grams.  An  hour  or  an  hour  and  a  half  after  giving  dye  vomiting  Bet 
in;  dog  lay  down  on  one  side  and  died  in  3  or  4  hours.  Cause  of  death, 
heart  filled  with  coagulated  blood;  lungs,  liver,  and  kidneys  filled  with  blood; 
turbid  swelling  of  the  liver  and  heart :  mucous  membrane  "t"  stomach  inflamed ; 
l>rain  unchanged.  Death  caused  l.y  paralysis  of  the  heart.  It  also  ads 
severely  on  the  skin. 

G.  T.  576. 

Tradr  names. — New  Gray;    Malta  Gray;  Nigrosin;  Direct  Gray; 
Methylene  Gray ;  New  Methylene  Gray, 

Scientific  name. —  (?) 

Discovered. — 1888. 

s/i<i<h . — Gray.     N<»t  offered. 

i  \\  OSABl  I. 

l.  Oblopzm  (/>.  "'''  examined  this  color,  and  on  his  own  experiments  concludes  it 
contains  '"no  poisonous  properties  "    The  experimental  data  follow  : 


136 


COAL-TAR    COLORS    USUI)    IN    FOOD   PRODUCTS. 

Experimental  data  ly  Chlopin. 
[1  gram=77  ing=.">4  grains.] 


Date.         Dose.       Weight.    **™* 

General  condition  of  animal  and  urine. 

1902. 
Feb.     8 
9 

Grants.         Kilos.            cr. 

3            12.9              510 

4«n 

Dm  quite  well;  urine  quite  normal. 
Urine  green  color;  acid;  no  albumen. 

Do. 

Do. 

Do. 
Vomited  once;  mine  dark  green;  acid;  no  albumen. 

Do. 

Do. 
Urine  lighter  shade. 

10 

11 

12 

13 

3 
3 
3 

3 
3 
3 

400 

450 

475 

14 
IS 
16 

"i.'.'.s 490' 

]7 

47.") 

Urine  normal;  dog  well. 

Total  . 

21 

G.  T.  584. 

Trade  names. — Safranin;  Safranin  S;  Safranin  cone;  Safranin 
GOO;  Safranin  T;  Safranin  extra  G;  Safranin  FF  extra;  Safranin 
AG,  AGT,  and  OOF. 

Name  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Safranin  SP. 

Scientific  name. — Mixture  of  diamhlo-phenvl-and-tolyMolazonium 
chlorids. 

Discovered  and  patented. — 1859. 

Shade. — Reddish  brown.     Offered  bv  1  out  of  12  sources. 


FAVORABLE. 


1.  Cazeneuve  (Arch.  gen.  tie  mid.  1886,   Vol.  I, 
disturbances  but  is  not  a  violent  poison. 


p.  753):  Produces  gastrointestinal 


(    \  FAVORABLE. 


1.  Prohibited  by  Confectioners'  List. 

2.  Wf.yl  (p.  SI):  "Caaeneuve  and    I  .opine  pointed  out  the  poisonous  nature  of 

*    *    *    Sairanine." 

3.  "This  body  (Chamber  of  Commerce  of  Soonebecg)  recommends  for  the  prepara- 

tion of  children's  toys  tlir colors,  the  poisonous  character  of  which  1  can 

demonstrate.     These  arc    *    *    *    Safranine    *    *    *  .    (p.  34.) 
A.  W'kvi,  (Handbueh  der  Hygiene):  "According  to  Theodore  Weyl  this  is  even  in  small 
doses,  when  injected  Bubcutaneously,  a  strong  poison"  (60  milligrams  per  kilo 
body  weight,  or  35  grains  per  LOO  pounds);    "whereas,  when  administered  by 
tlic  stomach  onlj  large  doses  over  a  long  period  of  time  produce  diarrhea." 
5.  Lbwim  (Lehrbuch  der   T<mkologiet   1897,  p.   132)    ''Safranin    is   poisonous  when 
injected  intravenously      (Pulse  acceleration,  dyspnoea,  cramps.)     Fed  to  dogs 
by  tin-  mouth  il  causes  only  diarrhea.'1 
Prohibited  by  the  Resolutions  ol  the  Society  o£  Swiss  Analytical  chemists,  of 

September,  L891. 
Prohibited  by  the  Canton  of  Tessin. 
i;i  si  Lists  it  as  poisonous. 
B    I  \/i  m  i  .i    \m-  1  i  ran     Compt.  rend.  1886,  v.  101,  p.  toil):  A  dog  (weight  not 

ran,  by  the  mouth,  daily  doses  of  from   I   to   l  j-ams  for  several 

only  salivation  and  diarrhea  were  produced.    They  conclude  that  it 

i-  a  harmful  color. 


COMPILED   DATA    UNDER    GBEEN    TABLE    NUMBERS.  137 

DOUBTFUL. 

1.  Winogradow  (Zts.  Nahr.  Genussm.,  1903,  v.  6,  p.  589)  says  it  almost  com- 
pletely inhibits  digestion. 

G.  T.  593. 

Trade  names. — Mauve;   Mauvein;   Chrome  Violet. 
Obsolete  nanus. — Mauve   Dye;    Anilein;    Anilin   Purple;    Violein; 
Indisin. 
Scientific  name. — Salts  of  phenyl-  and  tolyl-eafranins. 
Discovered  and  patented. — 1856. 
Shade. — Blue,  Reddish  Blue,  Bluish  Violet.     Not  offered. 

FAVORABLE. 

1.  Permitted  by  Confectioners'  List. 

G.  T.  599. 

Trade  names. — Indulin,  spirit  soluble;  Indulin  opal;  Fast  Blue  R 
and  B,  spirit  soluble;  Indulin  3B  and  6B,  spirit  soluble;  Indulin  3B 
opal;  Indulin  6B  opal;  Azin  Blue,  spirit  soluble;  Indigen  D  and  F; 
Printing  Blue;  Acetin  Blue. 

Scientific  name. — Mixtures  of  dianilidoamido,  trianilido  and  tetra- 
anilido  phem  1-phenazonium  chlorids. 

Discovered  and  patented. — 1863. 

Shade. — Blue.     Xot  offered. 

FAVORABLE. 

1.  Santo  in  {MolcachotV*  Untersuchungen,  1895,  v.  15,  p.  50):  A  dog  weighing  4,600 
grama  received  L2.5  grama  of  this  dye  (in  oil  I  in  :'.<>  days,  which  amounts  t<>  91 
milligrams  per  kil<>  per  day,  or  01  grains  per  LOO  pounds  per  day.  There  was  no 
disturbance  o!  any  kind.  Killed  by  chloroform;  autopsy  showed  everything 
to  be  normal. 

G.  T.  600. 

Tradi  nanus. — Nigrosin,  spirit  soluble;  Coupler's  Blue;  Oil  Black; 
Sloelin;  Spirit  Black. 

Scientific  name. — Mixtures  of  Iiuhilins  with  allied  bases  and  fluorin- 
dins. 

I>  icovered  and  patented.     ls<'»7. 

Shade.— Black.     Nol  offered. 

i  \\  ORABLK. 

I    Permil '<•<!  b)  ( onfectionera'  I  tat 

G.  T.  601. 

Tradi  name*. — Indulin, soluble;  Endulin3B;  Fast  Bin*'  Rand3R; 
Sloelin  RS  and  BS;  Indulin  R  andB;  LndulinGB;  Fast  Blue  2R,  B, 
and  6B. 


138 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Scientific  name. — Mixtures  of  the  sodium  salts  of  the  sulphonic 
acids  of  the  various  spirit-soluble  indulins. 
Discovered  and  yatented. — 1867. 
Shade. — Bronzy  or  Blue  Black.     Offered  by  1  out  of  12  sources. 


FAVORABLE. 

1.  Chlofln  (})p.  198-9):  On  his  own  experiments  classifies  this  color  as  nonpoisonous. 

The  experimental  data  are  as  follows: 

Experimental  data  by  Chlopin. 
No.l. 

[1  gram=">4  mg=  38  grains.] 


Date. 

Dose. 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

1902. 
Jan.     5 
6 

Grams. 
3 

Kilos. 

18.4 

cc. 
650 
670 
400 
410 
400 
400 
500 
560 
650 
620 

Dog  and  urine  normal. 

Urine  brown;  acid;  no  albumen. 

7 

3 
3 
3 
3 
3 

Urine  greenish  brown;  no  albumen. 
Do. 

g 

9 

Do. 

10 

Do. 

11 

Do. 

12 

Do. 

13 

Do. 

14 

Color  and  composition  of  urine  normal;  dog  is  well. 

Total  . 

18 

No.  2. 

[1  gram=114  mg=80  grains.] 


1902. 
Jan.  14 
15 
16 
18 
19 
20 
21 
22 
23 
24 
25 
2(1 

Total  . 


a 

3 
3 

8.8 

420 
390 

420 

3 
3 
3 

8.8 

400 

460 
400 
450 
4<X> 

18 

Dog  and  urine  normal. 

Urine  slightly  blue;  acid;  no  albumen. 

Do. 

Do. 
Urine  almost  normal  color;  no  albumen. 
Color  and  other  properties  of  urine  normal. 
No  record. 
I 'line  slightly  bluish;  no  albumen. 

Do. 
Dark  green;  no  albumen. 
Feeble  green;  no  albumen. 
Urine  normal;  dog  well. 


UNFAVORABLE. 

Santori  (MolcschoWs  Untertuehungen,  1895,  v.  15,  p.  55):  A  dog  weighing  4,500 
grams  received  4  to  (>  grams  dye  in  7  days,  which  amounts  to  ]27  to  100  milli- 
grams per  kil'>  per  day,  or  89  to  133  grains  per  100  pounds  per  day.    No  vomiting. 

Stool  black  hi  nc  and  no  change  in  the  urine.  Up  l<>  the  sixth  day  the  animal, 
in  very  good  general  condition,  ate  heartily  and  was  quite  lively;  temperature 
Unchanged  ,     On  the  morning  of  the  sixth  day  the  animal  was  found  in  his  cage 

Buffering  from  general  muscular  cramps  which  were  heightened  by  the  slightest 
noise;  the  animal  did  not  respond  to  calls  or  threatening  movements  and  was  in 
a  complete  stupor.    This  continued  for  24  hours,  when  the  animal  died.    Tho 

autopsy  showed  numerous  punctures  of  I  he  lungB  and  of  the  mucous  membrane 

of  the  stomach;  Eatty  degeneration  of  the  liver  and  little  blood  in  it;  kidneys 

without  change,  although  the  COrtei  wai  colored  a  light  green. 


COMPILED    DATA    UNDER    GREEN    TABLE    NUMBERS. 

G.  T.  602. 


139 


Trade  names. — Nigrosin,  soluble;  Bengal  Blue;  Gray  R  and  B. 
Scientific  name. — Sodium  salts  of  sulphonic  acids  of  spirit   nigro- 
sins. 

Discovered  and  patented. — 1867. 
Shade. — Black.     Not  offered. 


Nothing. 


FAVORABLE. 


UNFAVORABLE. 


1.  Lewin  (Lehrbuch  der   To.rikologie,  1897,  p.    931)  Bays:   "Produces  eczema,"  and 
cites  Deutsche.  Med.  Woehenschr.,  1891,  page 4~>- 

G.  T.  614. 

Trade  names. — Magdala  Red;  Naphthalene  Rose;  Sudan  Red; 
Naphthalene  Red;  Naphthylamin  Fink. 

Scientific  name. — Mixture  of  amido-naphthyl-naphthazonium- 
chlorid  and  diamido-naphthyl-naphthazonium  chlorid. 

Discovered. — 1868. 

Shade. — Red.     Not  offered. 


Nothing. 


FAVORABLE. 
UNFAVORABLE. 


1.  Chlofin  (p.  100)  examined  this  color,  and  on  his  own  experiments  concludes  it 

"does  not  belong  to  the  poisonous  list,  but  is  not  wholly  harmless."     The  ex- 
perimental data  are  as  follow-; 

/  zperimental  data  by  Cfdopin. 

No.  1. 

[t  gram— 91  mg— 64  grains.] 


D  . 

Weight. 

24  hours' 
urine. 

General  condition  of  animal  ;m<i  urine. 

Apr.    12 
13 
11 
15 

is 

- 

2 

A- 

Hot. 

it 

cc. 
1,100 

670 

Before  ezperimenl  dog  and  urine  normal. 
ise-oolored;  acid;  no  albumen. 
D  i 
Urine  quite  red:  acid;  no  albumen;  vomited  once. 
11;  mine  normal  In  color 
sttlon. 

;i!e 

eoinpo- 

Total 

•"' 

(l  gram    111 


: 

4 

.mi 

■  ni  i|iiii  •■  well;  mine  normal  ei>l«.r:  ;i«  il;    no 

line- 
Ill  the  morning  thm<  limes  thin  sIik»i,  urine  f.unii 

1;  no  albumen.   • 

■ 

7 

i 

Do 

| 

Do 

16 

140 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

Experimental  data  by  Chlopin — Continued. 
[1  gram=114  mg=80  grains.] 


Date. 

Dose. 

Weight. 

2  iirire^  i                      General  condition  of  animal  and  urine. 

1903. 
Feb.  10 

Grams. 
3 

Kilos. 

cc. 
310 

315 
350 

n 

muriatic  acid  rose  color,  becomes  greenish  gray. 

12 

8.8 

Xo  vomiting;  no  diarrhea;  color  reaction  of  urine  normal;  no 

albumen. 

Total  . 

3 

DoriiTIl  I. 


1.   Wixogradow  (Z/.s.  Nahr.  Genussm.  l(.)0.$,  v.  6,  p.  589)  says  it  almost  completely 
inhibits  digestion. 

G.  T.  620. 

Trade  names. — Gallocyanin  DII  and  BS;  Fast  violet;  GallocyaniD 
RS,  BS,  and  D. 

Scientific  name. — Dimethylamido  dioxy  phenazoxoniumcarboxy- 
late.     (BS  is  the  bisulphite  compound.) 

Discovered  and  patented. — 1881. 

SJiade. — Bluish  Violet.     Not  offered. 


Nothing. 


KAVOKAHI.K. 


UNFAYOKAB1.E. 


1.  Sastori  ( MoleschoW s  Untersuchungen,  1895,  v.  15,  p.  51):  A  Jog  weighing  5,400 
grams  received  7.5  grams  dye  in  30  days,  which  amounts  to  4G  milligrams  per 
kilo  per  day  or  32  grains  per  100  pounds  per  day.  Throughout  all  the  time 
the  animal  remained  well,  had  good  appetite,  temperature  normal,  no  Loss  of 
weight;  urine  and  feces  colored  deep  blue  black.  Killed  by  chloroform. 
Autopsy  showed  incipient  fatty  degeneration  of  the  liver  and  a  swelling  of  the 
kidneys.     Conclusion:    Poisonous. 

G.  T.  639. 

Trade  names.— Meldola's  Blue;  Cotton  Blue  Rj  Fasl  Navy  Blue 
R;  Naphthol  Blue  R  and  J);  Naphthylene  Blue  R  in  crystals;  Fast 
Blue  K,  2  R  and  3  R  for  cotton  in  crystals;  Fast  Navy  Blue  KM 
and  MM. 

Scientific  name. — Zinc  double  chlorid  of  dimethylamido-naphtho- 
phenoxazonium  chlorid. 

Discovered . — 1 8  7 (.  I . 

Shade.— Dark  Violet.     Not  offered. 


Nothing. 


I    \\<H<  \ltl.K 


I    MKAVOH  Mil  l 


1,  Chlopin  (pp.  194  195)  on  his  own  experiments  reports  this  color  as  "verj  poison- 
ous."   The  experimental  data  are  as  folio* 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 


141 


Experimental  data  by  Chlopin. 
No.  l. 
|1  gram=68  mg=48  grains.] 


Date. 


Dose. 


24  hours' 
urine. 


General  condition  of  animal  and  urine. 


1902.     i 
Jan.  5...: 


Total 


Grams. 


Kilo*. 
14.6 


S9Q 


Before  experiment  do,*  quite  well;  urine  normal  in  color  and 
composition:  1  hour  after  giving  the  dye  vomiting  began: 
dog  lay  down  on  ground  and  died  in  1  hour. 


No. 


[l  gram° 


mg    117  grains.] 


1902. 
Jan.    14 


15 
Total. 


3    

0 


Soon  after  giving  dye,  strong  vomiting  and  diarrhea;  after  a  few- 
hours  improved. 

Most  violent  vomiting;  dog  lay  down  on  his  side,  and  was  found 
dead  in  G  hours. 


Note.— See  p.  181. 

2.  Santori  (Mok.svhott's  Untersuchungeti,  1895,  v.  15,  p.  49):  A  dog  weighing  4,.~>0(i 
grams  received  12.5  grams  dye  during  30  days;  this  amounts  to  93.3  milligram* 
per  kilo  per  day  or  65.3  grains  per  hundred  pounds  per  day.  Continued  vom- 
iting beginning  with  0.2  grams  dye,  anaemia  and  copious  as  well  as  continuous 
salivation  and  emaciation;  the  animal  lost  1,200  grams  in  weight  or  27  per 
cent.  Killed  by  chloroform;  autopsy  showed  no  fat,  flabby  muscles,  stomach 
contracted  and  filled  with  mucous  and  in  part  colored  pea  green;  fatty  degen- 
eration of  the  liver;  contracted  bladder;  kidneys  swollen  and  congested  with 
blood  and  decomposed  blood  corpuscles  in  the  Bowman  capsules. 


G.  T.  649. 


Tradenames. — Gentianin;  Gentians  Violet 
Scientific  name. — Zinc   double   chlorids   of 
nazthionium  chlorid. 

Discovered  <m</  patented.—-  1886. 
Shadi .  -Violet.     Not  offered. 


iincl  1 


lyltliiimido  |>he- 


Nothing. 


PAVORABl  B. 


t    \i  A\ OKA  HI  I 


l.  Santorj  i  MolfchotV*  UnUrtuchungen,  1895,  v.  IS,  p  -.  :  \  dog  w<  ighing  3,008 
grama  received  4.7  grams  of  dye  in  7  days,  which  amounts  to  22 1  milligrams  jht 
kilo  per  day  or  157  grain-  per  LOO  pounds  per  day.  Beginning  with  the  third 
day  tii.'  dog  appeared  weak  and  depressed  and  ■  whitish  troth  appeal 
the  mouth;  mild  diarrhea  and  complete  aversion  to  food;  temperature  and 
urine  unchanged.  Died  on  seventh  day.  Autopsy  showed  congestion  «/ 
mucous  in.  iic  machj  the  liver  was  inflamed  and  the  kidneys  Btrongl] 

congested. 


142        COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

G.  T.  650. 

Trade  names. — Methylene  Blue  B  and  BG;  Methylene  Blue  BB  in 
powder  extra  D;  Methylene  Blue  BB  in  powder  extra;  Methylene 
Blue  A  extra. 

Names  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  in  1907. — Methylene  Blue  B;  Methylene  Blue. 

Scientific  name. — Chlorid  or  zinc  double-chloric!  of  tetramethyl- 
diamido-phenazthionium . 

Discovered. — 1876. 

Shade. — Blue.     Offered  by  2  out  of  12  sources. 

1AVORABLE. 

1.  Schacherl  (p.  1046):  "To  these  groups  belong  the  much-used  Methylene  Blue, 

which  in  moderate  doses  is  harmless." 

2.  Fraexkel  (p.  574):  "*    *    *    Methylene  Blue  causes  no  noteworthy  disturb- 

ances." 

3.  Cazexeuve  (Arch.  gen.  de.  med.  1886,  v.  1,  p.  753)  says  that  it  produces  gastric 

intestinal  derangements  but  is  not  a  violent  poison. 

unfavorable. 

1.  Prohibited  by  Confectioners'  List. 

2.  Weyl  (p.  31):  "Cazeneuve  and  Lepine  pointed  out  the  poisonous  nature  of 

*    *    *    Methylene  Blue    *    *    *." 

3.  Fraenkel  (p.  579):  "To  regard  Methylene  Blue  as  a  specific   remedy  BUch  as 

quinin,  is,  in  spite  of  a  few  such  experiments,  improper;  it  produces  sub- 
sidiary effects  which  depend  in  part  upon  local  irritation  of  the  intestinal  tract , 
and  partly,  however,  upon  irritation  of  the  bladder  with  increased  micturi- 
tion." 

4.  Cazexeuve  (Arch.  gen.  de  med.  1886,  v.  1,  p.  753),  says   that  it  produces  gastric 

intestinal  derangements. 

5.  Combemale  and  Francois  (Sem.  Med.  1890,  no.  31,  p.  258),  say  that  it  produces 

intestinal  disorders  and  vomiting,  colored  urine,  and  colored  feces  in  dogs, 
and  therefore  is  a  highly  injurious  color. 

6.  Saxtori  (Molcschott's  Untersuchunge?i.  1S95,  r.  15,  p.  4  J)  classes  it  as  injurious.     A 

dog  weighing  1,000  grams  received  in  20  days  18  grams  dye,  which  amounts  to 
196  milligrams  per  kilo  per  day,  or  137  grains  per  100  pounds  jht  day.  Urine 
and  feces  colored;  diarrhea  and  continuous  vomiting;  blood  and  pus  contained 
in  stool;  loss  of  appetite;  loss  of  weight  was  1 ,000  grams,  or  :r>  per  cent.  Animal 
died.  Autopsy  disclosed  blue-colored  skin  and  kit;  brain  turned  blue  on 
exposure  to  air,  but  only  the  outer  cortex  was  colored;  Btomachical  catarrh; 
the   mucous   membrane  of   the  stomach   colored   blue;   the  heart   sac   and   the 

pleura  colored  blue  to  blue-green;  Intestines  externally  blue;  kidneys  were 
thickened  and  colored  dark  blue  throughout;  parenchymatous  kidney  inflam- 
mation; fatty  degeneration  of  the  liver;  diaphragm  Locally  colored. 

7.  Aki.oivo  and  Cazbneuve,  quoting  Caceneuve  and  Lepine  (Arch,  de  med.  v.  9, 

p.  564 ',  Bay  thai  it  is  not  inactive. 

8.  Forbidden  by  Resolutions  of  Swiss  Analytical  Chemists,  September,  1891. 


COMPILED    DATA    UNDER    GREEN"    TABLE    NUMBERS.  143 

9.  Galliard  (Rev.  intern,  des  falsifications;  abst.  Hygien.  Runsdach.  1892,  p.  104)'- 
"  Methylene  Blue,  which  is  frequently  used  for  coloring  foods,  can  cause,  even 
in  small  doses  (10  to  20  milligrams,  or  one-sixth  to  one-third  of  a  grain),  a  feel- 
ing of  general  depression,  nausea,  and  certain  feelings  of  pain,  and  can  even 
produce  transitory  albuminuria.  In  larger  doses  (40  to  60  milligrams,  or  mx- 
tenths  to  nine-tenths  of  a  grain),  it  causes  in  the  case  of  persons  not  accustomed 
thereto,  vomiting,  diarrhea,  increased  micturition,  and  albuminuria.  In  the 
case  of  persona  suffering  from  nervous  diseases,  it  frequently  produces  disturb- 
ance which  has  as  its  consequence  a  cessation  or  a  change  of  place  of  the  pain 
Sometimes  it  produces  pain]  ing  of  pain  in  the  patient,  for 

which  no  certain  therapeutic  indication  could  be  determined." 

10.  Weyl  (Ila/tdbuch  drr  Hygiene)  comments  as  follows  "These  statements  of  Gal- 

liard arouse  but  little  confidence,  because,  as  is  well  known.  Methylene  Blue 
Lb  very  frequently  administered  to  invalids  in  doses  of  more  than  0.5  gram 
without  any  noticeable  disturbance.  Perhaps  Galliard 'a  preparation  was 
unclean.  At  any  rate,  in  all  experiments  on  the  poisonous  nature  of  Methylene 
Blue  it  is  to  be  considered  that  it  frequently  occura  in  commerce  as  a  zinc 
chlorid  double  salt." 

11.  Lewin  {Lehrbuch  dcr  Toiilologie,  1897,  p.  232):  "Methylene  Blue    *    *    *    can 

produce  after  prolonged  administration  of  0.5-1.5  gram  daily  increased  micturi- 
tion, irritation  of  the  bladder,  blue  coloration  of  the  urine,  and  .-aliva,  diarrhea, 
headaches,  vertigo,  delirium,  and  twitching  of  the  muscles,  the  latter  symp- 
toms probably  because  the  coloring  matter  is  deposited  in  the  brain." 

12.  Buss  tiste  it  as  poisonous. 

G.  T.  651. 

Trade  name. — Methylene  Green  G  cone,  extra  yellow  shade. 
Scientific  name. — Xitromethvlene  Blue. 
Discovered  and  patented, — 1SS6. 
Shade. — Green.     Not  offered. 


Nothing. 


FAYORAHI.F. 


•  VOHAHl.K. 


1.  (hi. <>ri\    pp  examined  this  color,  and  on  his  own  experiments  concludei 

ii  is  "non  poisonous,  but  somewhat  suspicious.'1    The  experimental  data 
are  as  toll 

•   inu  ntal  data  by  <  'hlopin. 

Nn.  I. 

ins.) 


'         '.    ^JSe?'  Imaland  urine. 


1901.        Oram*.       h  ii 

h  -  li:  urine  m 

i  rlne  dai  k  .  no  albumen. 

bumen. 

i  rlne  dark  brown;  no 
M  <8fi 

l    -;.  :  n<  ■ 

Total  .  •* 


144 


COAL-TAR    COLORS   USED   IN    FOOD   PRODUCTS. 
Experimental  data  by  Chlopin — Continued. 

No.  2. 
[1  gram=122  mg=X5  grains.] 


Date. 

Dose. 

Grains. 
3 

! 

3 

3 

Weight. 

urine*                          General  condition  of  animal  and  urine. 

1901. 
LVov.  25 
26 

Kilos. 
8.2 

cc. 
430 
445 
450 
410 
440 

Dog  well;  urine  normal. 
Urine  strongly  green:  no  albumen. 
Do. 

27 

:::::::::: 

28 

29 



Diarrhea;  urine  green:  acid;  no  albumen. 

Hec.  12 

Color  normal:  acid:  no  albumen:  dog  lively  and  well. 

Total. 

15 

DoriiTI-'l  I.. 


1.  Win'ogradow  (Zts.  Nahr.  Genussm.,  1903,  v.  6,  />,  It  noticeably  retards 

digestive  action;  is  not  indifferent . 

G.  T.  654. 

Trade  name. — Toluidin  Blue  O. 

Scientific    name. — Zinc-double-chlorid    of    dimethvl-diaiuido-tolu- 
phenazthonium-chlorid. 

Discovered  and-  patented. — 1888. 
Shade. — Blue.     Not  offered. 


Nothing:. 


FAVORABLE. 


UNFAVORABLE. 


I.  Fraenkel  (p.  374)'.  "Toluidin    Blue     *    *    *    is    a    strong    poison    for   micro- 
organisms, and  may  be  used  in  eye  treatment,  like  Methylene  Blue." 

G.  T.  659. 

Tradi  names. — Primulin;  Thiochromogen;  Sulphin;   Polychromin; 

Aurcolin. 

Scientific  name. — Sodium  salt  of  the  mono-sulphonic  acids  of  the 
dehydrothionated  condensation  products  of  dehydrothiotoluidin 
(mixed  with  some  sodium  dehydrothiotolwdin-eulphonate). 

Discovered.  —1887. 

Shade. — Yellow.     Not  offered. 


Nothing. 


I   W  ORABLE 


I  MA\  oi;  M.I  I 


I    Chlopin  (p.  103)  ex/unined  this  color,  and  on  his  own  experiments  reports  it  as 
'rapicious."    The  experimental  data  are  as  follows: 


COMPILED   DATA    UN  DEB    GREEN    TABLE    NUMBERS. 
Experimental  data  by  Chlopin. 

[I  gram=154  mg=l()S  grain.-.] 


145 


Date. 

Dose. 

Weight. 

24  hours" 
urine. 

(Sonera!  condition  of  animal  and  urine. 

1902. 
Mar.   21 
22 
23 

Grams. 
2.0 

id 

Kilos. 
0.5 

cc. 
292 
294 
355 
200 

Dog  and  urine  normal. 

Urine  dark  brown:  insignificant  traces  of  albumen;  acid. 

24 
25 

i  0.  o 

0.3 

L'rine  dark  brown;  acid;  no  albumen. 
Do. 

20 

No  albumen:  dark-brown  color:  dog  has  lassitude;  does  not  eat 

bread  nor  take  milk,  only  a  little  meat. 
No  albumen;  dark-brown 'color;  dog   has   lassitude;  dotj   eats 

little. 
At  the  point  of  injection  an  abscess  appears;  urine    . 

albumen;  yellow  color. 
Urine  acid;  no  albumen;  yellow  color:  dot;  eats  more. 

27 

291 

28 

29 

270 

280 

30 

Apr.     2 

Urine  normal:  appetite  almost  normal. 

Total  . 

1        '5.0 
{        .0., 

1  liv  mouth. 


-  Subcutaneously. 


al*o  Chlopis  (Zts.  NaJir.  Genuasm.,  t902,  v.  5,  p.  ?41). 


I><)  l    IJTFt    1 


I.  Winogradow    Zts.  Nahr,  Genussm.,  19Q3,  v.  6*,  p.  589)  says  ii  noticeably  retards 
digestive  action;  lw<>\  indifferent. 

G.  T.  667. 

Trad*   names.   -Quinolin  Yellow;    Quinolin  Yellow,  water-soluble. 

Narru  under  which  it  was  offered  on  the  United  States  market  as  a 
food  color  t/i  1907. — Ckinolin  Yellow  O. 

Scientifr  name. — Sodium  salt  of  the  Slllphonic  acid  (chiefly 
disulphonic  acid)  of  quinophthalone. 

Discovered.     1882. 

Shade. — Greenish  Yellow.     (Ml'crcd  by  1  out  of  12  source 


Nothing. 


I'AVOKA  BL1 


i\  I  A  \  ()lt.\  BL1 


I    Chlopin  (p.  W5 1  on  his  own  experiments  reports  this  color  as  "suspicious."     Tho 
experimental  data  arc  as  follow.-: 

ital  data  by  t  'Mopin . 

No.  l. 
[i  gram     ii  tng    81  gralna  | 


Jl  hours' 
iinm-. 

'..-n.-ial  condition  «.f  :m;in:il  :md  HI 

790 

•  experlmenl  dog  and  urine  normal 
i  rinc  .in  k  brown;  traces  albumen 
>l  uriiK-  normal;  do  albumen. 

•J  l 

97291°— Hull.  147   -12 10 


146  COAL-TAR    COLORS    USED    IN    FOOD   PRODUCTS. 

Experimental  data  by  rhlopin — Continued. 


Weight. 

24  hours' 
urine. 

General  condition  of  animal  and  urine. 

Mar.  23 

Grams. 
0.75 

Kilos. 
21.4 

cc. 

750 

Urine  dark  brown:  no  albumen. 
Dog  eats  nothing. 
Do. 

- 

603 

725 

5 

Do. 

27 

Dog  eats  nothing:  eats  poorly;  albumen  in  urine. 
Dog  eats  nothing;  rather  much  albumen. 

Do. 

30 

Do. 

Apr.     2 

Dog  eats  nothing;  traces  of  albumen. 

i  3.00 

710 

Color  of  urine  almost  normal;  insignificant  traces  of  albumen. 

Urine  yellow  brown;  traces  of  albumen;  appetite  normal. 

Trine  Yellow  brown:  no  albumen. 

- 

700 

Urine  and  dog  normal. 

Total. 

|      i  6.  00 
\     2  0.  75 

No.  2. 

[1  gram=  133  mg=*83  grains.] 


1903. 

Mar.     3 
4 
5 
6 

3.00 
3.00 
3.00 
2.00  , 

Total.. 

11.00 

320      Before  experiment  dog  quite  well,  and  urine  normal. 
300     Color  dark  yellow;  no  albumen;  general  condition  normal. 
300  I  Color  yellower  than  normal;  acid;  no  albumen. 
Do. 


1  By  mouth.  2  Subcutaneously. 

DOUBTFUL. 

1.  Wznooradow  (Zts.  Nahr.  Genussm.,  1903,  v.  6,  p.  589)  says  it  noticeably  retards 
digestive  action;  La  not  indifferent. 

G.  T.  670. 

Trade  names. — Vidal  Black;   Vidal  Black  S. 

Scientific    name. — Possibly    the    sulpho-hydro    derivative    of    a 
polythiazin. 

Discovered. — 1893. 

Shade. — Green.      Not  offered. 


Notl 
1.  Ch 


i \ VORABLB. 

i   \i  \  VOB  \  hi  i  . 


iiii'is  i />.  108)  examined  this  color,  and  on  his  own  experiments  classes  it  as 
■  very  harmful. "    The  experimental  data  are  as  follows. 

Experimental  data  by  Chlopin. 
[i  gram  - 132  mg    92  grains.] 


-' 

3 

_m  hours' 
urine. 

7.e 

890 

General  condition  of  animal  end  urine. 


i m.i 1 1  dog  quits  normal;  toon  altar  taking  dys 
vomited  tu  Ice. 
Qeneral  oondltion  good;  no  vomiting;  urine  turbid,  alkaline;  no 

albumen. 


COMPILED   DATA   UNDER   GREEX    TABLE    NUMBERS. 
Experimental  data  by  Chlopin — Continued. 


147 


Date. 

Dose. 

Weight. 

urine"*                         General  condition  of  animal  and  urine. 

1901. 
Dec.   31 

Grams. 
3 

3 

Kilos. 

cc. 

Vomited  soon  after  getting  dye;  appetite  less:  no  albumen. 
Urine  turbid;  scarcely  noticeable  blackisb  sheen;  green  with  sul- 

1902. 
Tan.     1 

2 

7 

358 

370 

phuric  and  hydrochloric  acid. 
Do. 

4 

3 
3 

Vomited  all  day  after  taking  dye;  eats  little:  no  albumen. 

5 

Violent  and  prolonged  vomiting  and  diarrhea;  condition  piti- 
able; further  giving  of  dye  stopped,  so  as  not  to  kill  the  animal. 
Vomiting  and  diarrhea  continue. 

5-7 

8 

Vomiting  and  diarrhea  stopped. 
Dog  is  livelier,  and  begin    to  eat. 
Dog  looks  well;  urine  normal  in  color;  acid;  no  albumen. 

9-11 

13 

Total.. 

17 

G,  T.  675. 

Trade  names. — Thiocatechin;  Thiocatechin  S. 
Shade.   -Brown.     Xot  offered. 


Nothii 


FAVORABLE 


UNFAVORABLE 


1.  Chlopin  (pp.   'in.  til    examined  this  color  and  classes  it  as  '"very  poisonous. 
Tl  •■  experimental  data  arc  as  follows: 

Experimental  data  by  Chlopin. 
[i  gram    12s nig— 90 grains.] 


General  condition  of  animal  and  urine. 


Dene. 

Weight. 

24  hours' 
urine. 

1902. 

Feb.  13 

14 

Grams. 
2.4 

2.0 

(I.:, 

Kilo*. 

7.S 

cc. 
300 

300 

u 

LI 

is 

4.9 

Before  experiment  dog  and  urine  quite  normal;  10  or  15  minutes 
after  giving  dye  dog  fell  on  one  side,  limbs  extended,  stomach 
drawn  in;  small  and  frequent  convulsions:  retching;  then 
abundant  vomiting,  same  color  as  dye;  soon  after  vomiting  dog 

got  up  and  walked  as  if  drunk;  hind  legs  tend  to  collaj. 

ration. 
a  few  minutes  after  giving  dye,  dog  again  fell  as  if  in  an  epileptic 
fit;  convulsions  of  the  extremities,  which  »  but  the 

dog  si  ill  lay  stretched  out,  with  open  eyes,  which  reacted  to 

light:  tongue  banging  out  to  one  side;  after  10  or  US  minutes 
vomiting  began;  dog  Mill  lying  on  one  Bide,  assumed  a  more 
normal  attitude:  15  minutes  later  dog  got  up.  walked  as  if 
drunk;  poor  control  over  hind 

Vomits  at  once  after  getting  dye,  but  remained  standing. 

Dog  appears  depressed,  bul 

Dog  quite  well;  urine  usual  normal  color:  no  albumen. 


Tradi  names, 

Sci<  itt'ific  nana 
Shade.     Blue. 


G.  T.  689. 

-Indigo;  Indigo  Pure  BASF. 
— [ndigotin. 

\<»t  offered. 


148 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


FAVORABLE. 

1.  Permitted  by  Confectioners'  List . 

2.  Permitted  by  the  law  of  Italy. 

UNFAVORABLE. 

1.  Fkaknkfl  (p.  oil):  "However,  pure  Indigo,  according  to  Robert,  is,  in  finely 

divided  condition,  a  violent  local  irritant." 


G.  T.  692. 

Trade  names. — Indigo  Carmine;  Indigo  Extract;  Indigotin. 

Xamrs  under  which  it  was  offered  on  the  United  States  market  as  a 
ft>od  color  in  1907. — Indigo  Carmine  Powder  IN;  Indigotin;  Indi- 
gol  ni  A. 

Scientific  name. — Sodium  salt  of  Indigotin  disulphonic  acid  or  the 
in-o  acid. 

Discovered, — 1740. 

Shade. — Blue.     Offered  by  3  out  of  12  sources. 

FAVORABLE. 

1.  Schacherl  (p.  1046):  "  No  objection  to  its  use." 

2.  Santori  ( .Volcschott's  Untcrsuchunyen.  1895,  v.  15,  p.  41):  A  dog  weighing  4,500 

grams  received  90  grams  dye  in  30  days;  vomited  twice  during  the  examina- 
tion; no  change  in  weight;  animal  killed  with  chloroform;  autopsy  showed 
-light  dull  swelling  in  the  epithelium  and  convoluted  canals  of  the  kidneys. 
This  dosage  amounts  to  6(!7  milligrams  per  kilo  per  day,  or  4G7  grains  per  100 
pounds  per  day.     Classes  it  as  harmless. 

ALPHABETICAL    INDKX    OF   TRADE    NAMES   OF   COAL-TAB    COLORS. 

The  following  list  of  the  trade  names  of  coal-tar  colors  appearing 
in  the  foregoing  compilation  on  physiological  action  is  complete 
when  supplemented  by  the  list  of  23  colors  given  on  page  227; 
Green  Table  numbers  in  parenthesis. 


A-  (tin  Blue  (599). 
Acid  Brown  (138). 
Arid  Green  I  134,435). 
Acid  Green  ex.  cone.  (435). 
Acid  ( rreen  cone.  I  135). 
Acid  Green  cone.  \'\  (435). 
Acid  Green  cone.  790  |  135). 
Acid  Fuchsin  ( 162). 
Arid  Magenta  I  162). 
Acid  Magenta  powd.  (462). 
Acid  Roeein  |  162 1. 
Acid  Rubin  I  162). 
Acid  Violel  I  W 
Acid  Violet  <i  B  (467). 
Acid  Yellow    - 

Arid    Yellow   AT  (1)1). 
Arid  Yellow  I)  (S8). 


Acid  Yellow  <i  (8). 
Arid  Yellow  (i  pat.  (8). 
Acme  Yellow  (84), 
Alizarin  Blue  ABS  (563 
Alizarin  Blue  S  (563). 

Alizarin  Green   527 1. 
Alphanaphthol  I  trange  (85). 
Alsace  Green  (394). 
Amaranth  ( L07). 

Amaranth  B  (10/ 
Anil,  in  (593). 

Anilin  Blue  Sp.  Sol. 
A ii il in  <  Grange  (2). 
Anilin  Purple  (593). 

Anilin  Bed  |  lis,. 
Anilin  Yellow  (1). 
Anilin  Yellow  8  (4). 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 


149 


Anthracene  Green  (527). 

Anthracene  Blue  S  (563). 

Archil  Substitute  V  (28). 

Atlas  Orange  (86). 

Auramin  (425). 

Auramin  O  (425). 

Aurantia  (6). 

Aureolin  (659). 

Aurin  (483). 

Azalein  (408). 

Azarin  S  (70). 

Azin  Blue,  spirit  soluble  (599). 

Azo  Acid  Rubin  (103). 

Azo  Acid  Yellow  (92). 

Azo  Blue  (287). 

Azo  Flavin  (92). 

Azo  Fuchsin  G  (93). 

Azo  Rubin  (103). 

Azo  Rubin  A  (103). 

Azo  Rubin  S  (103). 

Bavarian  Blue  DBF  (479). 

Bavarian  Blue  DSF  (478). 

Bengal  Blue  (602). 

Bengal  Green  (427). 

Benzoflavin  (530). 

Benzopurpurin  4B  (277). 

Betanaphthol  Orange  (86). 

Biebrich  Scarlet  (163). 

Bismarck  Brown  (197). 

Bismarck  Brown  R  (201). 

Bitter-almond-oil  Green  (427). 

Bleu  de  Nuit  (457). 

Bleu  Lumiere  (457). 

Bleu  Marine  (480). 

Bordeaux  B  (66). 

Bordeaux  B  L  (65). 

Bordeaux  R  ext.  (66). 

Bordeaux  8    L07). 

Brilliant  Black  B  (188). 

Brillaut  Cotton  Blue,  greenish  (479). 

Brilliant  Green    128 

Brilliant  Orange    L3 

Brilliant  Scarlet    L06 

Brilliant  Scarlet  IB    L06). 

Brilliant   Yellow 
Brilliant   Veil,.-. 
Butter  Yellow    L6 
Canary  Yellow    I 
I  larbasotic  Acid  (1). 

Cardinal  SB  (  I" 

Carminaph  I  1 1 

( "animism  |  L03 

Carmoisii]  B  i  LO 


Cerasin  (102). 
Cerasin  Orange  I  (11). 
China  Blue  (480). 
Chlorin  (394). 
Chrome  Violet  (593). 
Chrysamin  R  (269). 
Chrysaurein  (86). 
Chryseolin  (84). 

Chrysoidin  Crystals  (17,  18,  41). 
Chrysoidin  R  (17,  IS,  41). 
Chrysoidin  Y  (17,  18,  41). 
Chrysoin  (84). 
Chrysoin  REZ  (84). 
Cinnamon  Brown  (197). 
Citronin  (4). 
Claret  Red  (65). 
Claret  Red  RZ  (103,  106,  107). 
Ccerulein  S  (527). 
Cochineal  Red  A  (106). 
Congo  Red  (240). 
Cotton  Blue  (480). 
Cotton  Blue  R  (639). 
Cotton  Red  4B  (277). 
Coupler's  Blue  (600). 
Crocein  Orange  (13). 
Crocein  Orange  10234  (13). 
Crocein  Orange  G  (13). 
Crocein  Scarlet  (106). 
Crocein  Scarlet  3B  (160). 
Crocein  Scarlet  4BX  (106). 
Crocein  Scarlet  7B  (169). 
Crocein  Scarlet  8B  (169). 
Curcumin  (89). 
Curcumin  S  (399). 
Dahlia  (450,  451). 
Dark  Green  (394). 
Diamond  Green  B  (427). 
DianthinG  (511 
Dinitro-creaol  (2 
Dinitroeoreeorcin  (394). 
Diphenylamin  Blue 
Diphenylamin  orange  (88), 
Direct  Gray  (671 

\  iolet  (  r.i 
Emerald  Gn 
Emerald  ( rreen 
Engliab  Brown  (197V 
Eoan 

Bonn  A  (512). 
Boon  A  ei 

B    512). 

!  >17). 

Eoan  GG  i    512). 


150 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Eosin  J  (512,  517). 

Eojrin  10  B  (521). 

EoeiD  3J  &  4J  ext.  (512). 

Eocrin  Y  (512). 

Eo^in  Yellowish  (512). 

Erika  B  (78). 

Erythrobenzin  (448). 

Erythrosin  (517). 

Erythrosin  B  (517). 

Erythrosin  D  (517). 

Erythrosin  G  (516). 

Erythrosin  yellow  shade  (517). 

Ethyl  Green  (428). 

Fast  Blue  (477). 

Fasl  Blue  B,  spirit  soluble  (599). 

Fast  Blue  R  and  3R  (601). 

Fast  Blue  R,  spirit  soluble  (599). 
Fast  Blue2R,  B,  and  6B  (60! 

Fast  Blue  R,  2R,  and  3R  (639V 
Brown  G  (138). 

Fast  Green  (427). 

Fast  Green  J  (428). 

East  Green  O  (394). 

East  Myrtle  Green  (394). 

Fast  Navy  I'.lue  R  (639). 

East  Navy  Blue  RM  and  MM  (639). 
Ponceau  B  |  L6 

East  Red  (102,  105). 

Fasl  Red  C  (103). 

Fast  Red  D  (107). 

Fasl  Red  EB  (107). 

Fast  Violet  (620). 

Fellow  (4,8,  9,88). 

Fasl  Yellow  extra  (8). 
Yellow  G 

Fast  Yellow  053  (8;. 
Yellow  It  (9). 

Fine  Blue  (457). 

Fuchsiacin  (448). 

Fuchsin  I  I 

Fuchsin  cryst.  (448 

Fuchsin  8  (462). 

Gallocyanin  I'll  and  us  (620). 

Gallocyanin  lis.  BS,  and  D   I 

Gentian  Bluet 
tiana  Viol< 

I      ttianin  (64 

Gold  Orange   - 

Gold  Yellow  (84 

Golden  Yellon 
Rand  B   I 

Green  E 

G  sen  087    12* 

Guin< 


Harmalin  (448). 

ilelianthin  (87). 

Helvetia  Blue  (479). 

Hessian  Blue  (457). 

Hofmann  Violet  (450). 

Hydrazin  Yellow  (94). 

Imperial  Scarlet  (163). 

Imperial  Yellow  (6). 

Indigen  D  and  F  (599). 

Indigo  (689). 

Indigo  Carmine  (692). 

Indigo  Carmine  powd.  IN  (692). 

Indigo  extract  (692). 

Indigo  pure  BASF  (689). 

Indigotin  (692). 

Indigotin  A  (692). 

Indisin  (593). 

lndisinRandB(601). 

Indophenol  (572). 

Endophenol  white  (572  . 

Indulin  opal.  (599). 

Indulin  sol.  (601). 

Indulin,  spirit  soluble  (599). 

Indulin  3B  opal.  (599). 

Indulin  6B  opal.  (599). 

Indulin  3B%p.  sol.  (599). 

Indulin  6B  sp.  sol.  (599). 

Indulin  3B  (601). 

Indulin  6B  (601). 

Iodeosin  B  (517). 

[odeosinG  (516). 

Eodin  Green  (459). 

lodin  Violet  (450). 

Jaime  Acide  (4,  8). 

Jaune  Acide  C  (-1 >. 

Jaime  Xaphthol  (3). 

Jaune  d'Or 

Jaune  d'Orient  (516). 

Jaune  Soleil  (39 

Kaiser  Yellow 

Kermesin  Orange  (97). 

Leather  Brown  (197). 

Leather  Veil-, 

Lemon  Yellow  (4). 

Light  Green  8  F  bluish  (434). 

a  s  F  yellow  shade  |  135), 

London  Blur  extra 

Magdala  Red  (614). 

Magenta  <  148 

M  ,  pnta  I'  A  B  8  Red  (448). 

,ia  Powder  A  (448 
Maize  (399). 
Malachite  Green  (42' 
Malachite  Green  B  (427-428). 


COMPILED   DATA   UNDER   GREEN    TABLE    NUMBERS. 


151 


Malta  Gray  (576). 

Manchester  Brown  (197). 

Manchester  Brown  EE  (201). 

Manchester  Yellow  (3). 

Mandarin  G  R  (97). 

Mandarin  G  ext.  (86). 

Martius  Yellow  (3). 

Mauve  (593). 

Mauve  Dye  (593). 

Mauvein  (593). 

Meldola's  Blue  (639). 

Metanil  Yellow  (95). 

Methyl  Blue  water  soluble  (478). 

Methyl  Blue  for  silk  MLB  (478). 

Methyl  Blue  O  (479). 

Methyl  Violet  (451). 

Methyl  Violet  B  (451). 

Methyl  Violet  BB  ext.  (451). 

Methyl  Violet  3  BD  (451). 

Methylene  Blue  (650). 

Methylene  Blue  A  ext.  (650). 

Methylene  Blue  B  and  BG  (650). 

Methylene  Blue  B  D  (650). 

Methylene  Blue  BB  extra  (650). 

Methylene  Blue  BB  extra  D  (650). 

Methylene  Gray  (576). 

Methylene  Green  G.  cone.  ext.  (651). 

.Naphthalene  Pink  (614). 

Naphthalene  Red  (614). 

Naphthalene  Rose  (614). 

Naphthol  Black  B  (188). 

Naphthol  Black  BDF  (188). 

Naphthol  Blue  R&D  (639). 

Naphthol  Green  (398). 

Naphthol  Green  B  (398). 

Naphthol  Grange  (85). 

Naphthol  Red  S  (107). 

Naphthol  Yellow  (3,  4). 

Naphthol  Yellow  L  (4). 

Naphthol  Yellow  8  (4,5). 

Naphthol  Yell.,wSLOZ(4,86). 

Naphthylamin  Yellow  (3). 

Naphthylene  Yellow  (2). 

Navy  Blue  B 

New  <  loccin  (101 

New  Gh 

New  Green  I  12 

New  If  ethylene  Gray  (570). 

New  Red  L  |  Lfl 

\  ictaria  Green    r_':.428). 
New  Yellow  (88). 
New  Yellow  L   - 
Nicholson  Blue    177). 
Nigh!  Green  (460). 


Nigrosin  (576). 

Nigrosin  sol.  (602). 

Nigrosin  sp.  sol.  (600). 

Nitrodiphenylamin  (6). 

Nitromethylene  Blue  (651). 

Oil  Black  (600). 

Oil  Orange  7078  (11). 

Oil  Yellow  (16). 

Opal  Blue  (457). 

Orange  (86). 

Orange  I  (85). 

Orange  II  (86). 

Orange  III  (87). 

Orange  IV  (88). 

Orange  A  (86). 

Orange  A  extra  (86). 

Orange  Brown  (17,  18,  41). 

Orange  A  1201  (86). 

Orange  B  (85). 

Orange  extra  (86). 

Orange  G  (14). 

Orange  GG  (14). 

Orange  GG  Crystals  (14). 

Orange  GRX  (13). 

Orange  GS  (88). 

Orange  GT  (43). 

Orange  M  (88). 

Orange  MN  (95). 

Orange  N  (43,88). 

Orange  O  27  (85). 

ge  O  (43). 
Orange  R  (15,  55,  97). 
Orange  RN  (43). 
Orange  RZ  (85). 
Orange  T  (97). 
Orange  2  R  (97). 
Orange  Y  (86). 
Orcellin  No.  4  (102). 
Paris  Violet  (451). 
Phenylene  Brown  (197). 
Philadelphia  Yellow  G  (532). 
PhloxiinVj]  . 
Thloxin  T 
Phoepbin    5 
Picric  Add 

Polychromin  (660). 
Pomona  Gn 
Ponceau  B  (163). 
Ponceau  A  GB  (IS). 
Ponceau  4  KB 

mi  (.  and  (  .  R 

Ponceau  R 

;       ma  kb 


152 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Ponceau  2  G  (15). 
Ponceau  2  R  (55;. 
Ponceau  6  RB  (109,. 
Primula  (450  . 
Primulin  (6« 
Printing  Blue  (599;. 
Pure  Soluble  Blue  (480). 
Pyoctanin  Aureum  (425;. 
Pyoctanin  (451). 
Pj  rosin  B  (517). 
i\  r  -in  J  (516  . 

Quinolin  Yellow,  water-soluble  (667). 
Quinolin  Yellow  (667). 
Rauracienne  (102). 
Red  (107). 

Red  Violet  5  R  extra  (450). 
Resorcin  Yellow  (84). 
.■in  0  275  (84). 
Rhodamin  (504). 
Rhodamin  B  (504). 
Rhodamin  O  (504;. 
Rhodamin  B  extra  (504). 
Rhodamin  G  and  (i  extra  (502). 
Roccellin  (102,. 
Rose  Bengal  (520). 
Etoee  Bengal  AT  (520). 
Rose  Bengal  G  (520). 
Rose  Bengal  N  (520). 
I'    •••in  (448;. 
Rosolic  acid  (483). 
Rubianite  (448). 
Rubidin  (102  . 
Rubin  (448). 
Rubin  S  (402). 
Russian  Green  (394). 
Saffron  Substitute  (2). 
Saffron  Yellow  (3,  4). 
Bafranilin  (504). 
Safranin  (584). 

Safranin  AG,  A.GT,  and  OOF.  (584). 
Safraniii  Cono.  (584). 
Safranin  extra  <  I  1 58 1 

!.in  PF  extra  (584;. 
Safranin  GOO.  < 
Safranin  S.  (584). 
Safranin  SP 
Safranin  T     584 
Scarlet  (55). 

Scarlet   L.  (106). 

Sloelin  (600). 

Sloelio  RS.  and  BS.  (001). 

Solferino  (448 

Solid  bellow  i  i 

Soluble  Blue  |  L£ 

Spirit  Black  (600). 


Spirit  Blue  (457). 

Soluble  Blue  8  B.  (479). 

Soluble  Blue  10  B.  (479). 

Soluble  Blue  XL.  (479;. 

Succinic  (4). 

Sudan  I  (11). 

Sudan  Red  (614). 

Sulphin  (659). 

Sulphin  Yellow  (4). 

Sulphonaphthol  Acid  Yellow  (4). 

Sultan  Red  4  B.  (277). 

Sun  Yellow  (399). 

Tartrazin  (94). 

Thio  Catechin  (675). 

Thio  Catechin  S.  (675). 

Toluidin  Blue  O.  (654). 

Tropaeolin  D.  (87). 

TropaeolinG.  (95). 

Tropaeolin  O  (84). 

Tropceolin  OO  (88). 

Tropseolin  OOO  (85). 

Tropaeolin  OOO  No.  2  (86). 

Tropa?olin  R  (84). 

tfreol  D.  (574). 

Ursol  DD.  (574). 

Ureol  P.  (574). 

Vert  Diamant  (427). 

Vert  Lumiere  (459). 

Vesuvin  (197). 

Vesuvin  B.  (201). 

Victoria  Blue  B.  (488). 

Victoria  Blue  4  R.  (490). 

Victoria  Orange  (2). 

Victoria  Yellow  (2). 

Victoria  Yellow  Cone.  Z.  (95). 

Vidal  Black  (670). 

Vidal  Black  S.  (670). 

Violein  (593). 

Violet  de  Methylanilin  (451). 

Violet  R.  (450). 

Violet  RR.  (450). 

Violet  5  R.  (450). 

Water  Black  (166;. 

Water  Blue 6  B  extra  (ISO). 

Water  Blue  (180). 

Xanthin  (532). 

XL  Soluble  Blue  (479). 

Xylidin  Red  (55). 

Xylidin  Scarlet  (55). 

Yellow  Corallin  (483). 

Yellow  FY.  (4). 

Yellow  MXX  Cone.  (95), 

Yellow  W 

Yellow  Wit.  (89). 


DOSAGE   AND   SYMPTOMS.  153 

X.  DOSAGE  AND  SYMPTOMS. 
CONFECTIONERS'  LIST  AS  A  BASIS  FOR  A  RULE. 

Considering  the  Confectioners'  List  of  1899  as  a  correct  guide  as  to 
which  colors  are  harmful  and  which  are  harmless,  the  attempt  has 
been  made  to  determine  how  far  dosage  and  the  corresponding 
physiological  effects  may  serve  as  a  guide  in  determining  which  colors, 
other  than  those  enumerated  in  either  portion  of  the  Confectioners' 
List,  are  harmful  or  harmless.       (See  p.  48.) 

To  this  end  the  available  literature  has  been  searched  and  classified, 
and  wherever  it  was  possible  to  arrive  at  any  conclusion  as  to  the 
actual  dose  or  the  average  dose  over  a  stated  period  of  time,  and  the 
corresponding  physiological  observations,  these  data  have  been  sepa- 
rated and  brought  together  for  the  purpose  of  making  comparisons 
and  deductions  therefrom. 

It  wras  thought  that  the  literature  would  show  that  if  a  dog  or  other 
animal  is  killed  by  a  certain  given  amount  of  color  per  100  pounds  of 
body  weight  of  the  animal  that  such  color  is  always  harmful;  that  if 
untowTard  effects,  such  as  vomiting,  diarrhea,  weakness,  and  general 
depression,  are  caused  by  more  than  a  certain  weight  of  color  per  100 
pounds  body  weight  of  the  animal,  such  color  is  always  regarded  as 
harmless. 

The  classification  of  the  available  literature  and  the  conclusions 
therefrom  are  as  follows: 

Of  the  33  coal-tar  colors  listed  as  harmless  in  the  Confectioners1 
List,  10,  namely,  G.  T.  4,  9,  55,  65,  85,  103,  105,  107,  448,  and  462, 
have  been  tested  on  humans,  while  the  conclusion  as  to  the  remaining 
23  is  reached  by  the  effects  observed  on  dogs  alone.  However,  con- 
tradictory statements  are  recorded  in  the  case  of  No.  9,  and  none  of 
these  tests  was  of  long-continued  duration,  but,  on  the  contrary,  in 
many  cases  the  time  covered  was  exceedingly  short,  and  the  conclu- 
sions deduced  are,  therefore,  not  necessarily  final  nor  correct.  It 
should  he  further  noted  that  No-.  95  and  106,  reported  as  nonpoi- 
sonous  to  humans,  are  in  the  harmful  section  of  this  Confectioners' 
List . 

I.  Those  colors  which  produced  no  effect  are  as  follows  (the  num- 
ber of  grains  given  i-  the  amount  administered  per  100  pounds  body 
weight :  where  the  data  permitted,  the  number  of  days'  duration  of 
I  he  experiment  is  also  given : 

.    Brilliant  Fellow  8  

13.  Ponceau  4  GB LIS 

(21      TlilMxin 

521.  Phloxin BOO 


154         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

II.  Those  colors  which  in  some  cases  produced  no  effect,  and  in 
others  produced  effects,  are  as  follows: 

4.  Naphthol  Yellow 

395  grains  produced  diarrhea  and  no  albuminuria. 
292  grains  produced  albuminuria. 

116  grains  for  25  days  produced  no  effect. 

25  grains  for  2  weeks,  on  alternate  days,  produced  no  effect. 
8  and  9.  Fast  Yellow  Y  and  R: 

173  grains  for  3  weeks  produced  no  effect. 

53  grains  produced  albuminuria. 
55.  Ponceau  2  R. 

582  grains  killed. 

198  grains  produced  no  effect. 
05.  Fast  Red  B: 

143  grains  for  145  days  produced  no  effect. 

137  grains  for  145  days  produced  no  effect. 

98  grains  for  145  days  produced  no  effect. 

68  grains  produced  albuminuria. 

38  grains  produced  albuminuria. 
103.  Azorubin  S: 

143  grains  for  145  days  produced  no  effect. 

137  grains  for  145  days  produced  no  effect. 

98  grains  for  145  days  produced  no  effect. 

70  grains  produced  diarrhea. 
287.  AzoBlue: 

233  grains  produced  no  effect. 

166  grains  produced  albuminuria. 

III.  Those   that   produced   only  a  slight  disturbance  which  was 

regarded  as  negligible: 

28.  Archil  Substitute  V: 

301  grains  produced  vomiting  and  albuminuria. 

127  grains  produced  vomiting  and  albuminuria. 
105.  Fast  Red  E: 

70  grains  produced  diarrhea. 
166.  Wool  Black: 

117  grains  produced  albuminuria. 
240.  Congo  Red: 

192  grains  produced  albuminuria. 
269.  Chryaamirj  R: 

433  grains  produced  albuminuria. 

361  grains  produced  albuminuria. 
39 1.  Dinitrosoresorciii : 

L39  grains  produced  loss  of  appel  Ite. 

121  grains  produced  albuminuria. 

From  Class  1  above  it  would  appear — 

(a)  Thai  if  a  dose  of  1 13  grains  per  100  pounds  body  weight  pro- 
duced no  effect  it  is  to  be  classed  as  harmless. 

From  Class  II  above  Li  would  appear — 

(a)  That  if  albuminuria  is  caused  by  as  little  as  38  grains  in  some 
cases,  and  no  effect  is  produced  by  doses  as  large  as  14.'*  grains,  the 
volor  is  to  be  classed  as  harmless. 


DOSAGE   AND    SYMPTOMS.  155 

(6)  Also  that  if  198  grains  produce  no  effect  the  color  is  to  be 
classed  as  harmless,  even  if  582  grains  in  another  case  kill  the  animal. 

(c)  That  if  small  amounts  produce  albuminuria  and  larger  amounts 
do  not  the  color  is  to  be  classed  as  harmless. 

(d)  That  if  small  amounts  produce  diarrhea  and  larger  amounts 
do  not  the  color  is  to  be  classed  as  harmless. 

From  (lass  III  it  would  appear  that — 

(a)  Albuminuria  produced  by  as  little  as  1 1 7  grains  is  to  be  regarded 
as  not  harmful. 

(b)  Diarrhea  produced  by  70  grains  is  to  be  regarded  as  not  harmful. 

(c)  Vomiting  and  albuminuria  produced  by  127  grains  are  to  be 
regarded  as  not  harmful. 

The  colors  classed  as  harmful  in  the  Confectioners'  List  may  be 
classified  as  follows : 

I.  Dogs. — Those  colors  that  under  certain  conditions  produce  no 
noticeable  effects  on  dogs,  while  under  other  conditions  effects  are 
observed,  are  classed  as  harmful  colors: 

1.  Picric  Acid: 

Dogs  stand  5  grains  daily  for  18  days  without  effect. 
18£  grains  produced  diarrhea. 
20.4  grains  killed. 

2.  Dinitrocresol: 

140  grains  caused  vomiting  but  did  not  kill. 
38£  grains  caused  vomiting  but  did  not  kill. 
38£  grains  caused  vomiting  and  did  kill. 

35  grains  caused  vomiting  but  did  not  kill. 
31.6  grains  caused  vomiting  but  did  not  kill. 

3.  Martins  Yellow: 

51  grains  do  not  kill,  but  produce  weakness,  diarrhea,  and  albuminuria. 
50  grains  kill. 

8  grains  do  not  kill,  but  produce  weakness,  diarrhea,  and  albuminuria. 
B6.  Orange  II: 

71  1  trains  produced  kidney  irritation,  thirst,  and  diarrhea. 
333  grains  kill,  and  produced  diarrhea  and  albuminuria. 
244  grains  produced  kidney  irritation,  thirst,  and  diarrhea. 

36  grains  produced  DO  effect. 
a").  Itetanil  Yellow: 

620  grains  pr<>dnre  vomiting. 

803  grains  kill. 

m?  grains  no  effect , 

371  grains  kill. 

lot  grains  produced  albuminuria. 
tiL*  grains  no  effect 
•i  I  grains  do  effect , 
::i  grains  kill. 
i!»7.  Bismarck  Brown: 

2 16  grains  produced  vomit  ing. 
I  is  grains  produced  vomiting  and  general  depression. 
grains  daily  for  3o  days,  do  effect. 


156         COAL-TAB  COLORS  USED  IN  FOOD  PRODUCTS. 

398.  Naphthol  Green  B: 

600  grains  produced  green  urine  and  conjunctiva. 

292  grains  produced  no  effect. 

12S  grains  produced  green  urine  and  conjunctiva. 

II.  Those  colors  that   have  not  been  observed  to  give  negative 
results,  but  which  have  caused  certain  effects: 

11.  Sudan  I: 

118  grains  produced  colored  urine,  vomiting,  and  albuminuria. 
17  and  18.  Chrysoidin  Y  and  R: 

79  grains  produced  albuminuria. 

74  grains  for  30  days  produced  no  albuminuria,  but  a  loss  of  12 J  per  cent  of 
body  weight. 
88.  Diphenylamin  Orange: 

216  grains  produced  albuminuria. 

128  grains  produced  phenol  in  urine  and  albuminuria. 
138.  Fast  Brown  G: 

237  grains  produced  diarrhea  and  loss  of  appetite. 

218  grains  produced  diarrhea. 

III.  Rabbits: 

1.  Picric  Acid: 

24.5  grains  for  90  days,  no  effect. 

45  grains  for  19  days  kill. 
86.  Orange  II: 

292  grains,  no  effect. 

933 grains  kill. 
95.  Metanil  Yellow: 

216  grains,  no  effect. 

IV.  Humans: 

1.  Picric  Acid: 

8.3  grains  no  effect. 
13.8  grains  no  effect. 
Invalids  and  children  can  not  stand  this  color. 

2.  Dinitrocresol: 

42  grains  kill. 
86.  Orange  II: 

1£  grain.-,  no  effect. 

3  grains,  headache,  vertigo,  dryness  of  throat,  and  poor  general  condition. 
95.  Metanil  Yellow: 

1£  grains,  no  effect. 

3  grains,  n<>  effect. 

From  Classes  I  and  II  above,  it  would  seem  to  appear — 

(a)  That  if  a  dog  is  killed  the  Colof  is  harmful,  even  though  it  take  us  much  M  008 
.-Mm-,  or  aa  little  as  20.4  grains  per  LOO  pounds  body  weight  t<»  kill. 

(b)  That  if  albuminuria  is  produced  in  dogs  by  as  little  as  7!)  grains.  <>r  as  nnicli  M 

tins,  the  color  is  harmful. 

(c)  That  if  diarrhea  la  produced  in  dogs  by  as  much  aa  218  grains,  or  is  little  m  ">o 
as,  ih<-  color  is  harmful. 

(d)  That  even  If  a  dog  can  take  as  much  a.s  107  grains,  the  color  may  be  harmful. 


DOSAGE   AND   SYMPTOMS.  157 

From  Class  III  it  would  appear — 

(a)  That  even  if  rabbits  can  stand  as  much  us  292  grains,  or  as  little  as  24.5  grains, 
the  color  is  harmful. 

From  Class  IV  it  would  appear — 

(a)  That  if  42  grains  kill  a  human,  the  color  is  harmful. 

(6)  That  even  if  humans  can  stand  as  much  as  3  grains  without  untoward  effect, 
the  color  is  harmful. 

The  conclusions  that  may  be  drawn  from  these  data  are: 

1.  If  a  dog  is  killed  by — 

(a)  603  grains  per  100  pounds  body  weight,  the  color  may  be  harmful. 
(6)  582  grains  per  100  pounds  body  weight,  the  color  may  be  harmless. 

2.  If  a  dog  can  bear  without  effect — 

(a)  407  grains  per  100  pounds  body  weight,  the  color  may  be  harmful. 

(b)  198  grains  per  100  pounds  body  weight,  the  color  may  be  harmless. 

3.  If  albuminuria  is  produced  in  a  dog  by — 

(a)  38  grains,  or  143  grains  per  100  pounds,  body  weight  the  color  may  be  harm- 
less. 

(6)  79  grains,  or  128  grains  per  100  pounds  body  weight,  the  color  may  be  harm- 
ful. 

4.  If  diarrhea  is  produced  in  a  dog  by — 

(a)  70  grains  per  100  pounds  body  weight,  the  color  may  be  harmless. 
(6)  50  grains  per  100  pounds  body  weight,  the  color  may  be  harmful. 

5.  If  vomiting  and  albuminuria  are  produced  in  a  dog  by  127  grains  per  100  pounds 
body  weight,  the  color  is  not  necessarily  harmful. 

6.  If  small  amounts  of  color  produce  in  a  dog  diarrhea  or  albuminuria,  and  larger 
amounts  do  not,  the  color  may  be  harmless. 

7.  Even  though  rabbits  can  withstand  292  grains  per  100  pounds  body  weight,  the 
color  is  not  necessarily  harmless,  but  may  be  harmful. 

8.  If  42  grains  kill  a  human,  the  color  is  harmful. 

9.  If  a  human  can  withstand  3  grains  without  effect  the  color  is  not  necessarily 
harmless,  but  may  be  harmful. 

10.  If  a  human  can  not  withstand  3  grains,  even  though  it  can  withstand  1^  grains, 
the  color  is  not  necessarily  harmless,  but  may  be  harmful. 

Lehmann  I  Meihoden  der  praktischen  Hygiene,  1890,  p.  545)  says: 

I  regard  such  substances  as  harmful  to  health  which  when  fed  t<>  a  sound  dog  in 
doses  of  a  few  decigram^  per  day  produce  at  once,  or  after  a  few  repetitioni  of  the  dose, 
disturbance  in  the  health  of  the  dog;  on  the  other  hand,  dyes  which  in  doses  of  bom 

one  to  several  grams  can  be  taken  for  weeks  '>n  end  withoill  Causing  any  disturbance 
or  only  sli;_rlit  intestinal  disturbances  "r  a  slight  and  passing  albuminuria  can  bo 
regarded  a-  harmless,  h.  should  never  be  forgotten  that  a  few  milligrams  of  a  coal- 
tar  color  dyes  very  strongl)  and  it  a  not  easy  even  by  most  extraordinary  use  of 
colored  objects,  e.  g.,  by  children  that  more  than  milligrams,  at  most  centigrams, 
of  dye  can  he  introduced  into  the  human  Btomach.  In  extremely  large  doses  many 
substances,  for  example,  all  our  condiments,  are  naturally  harmful. 

Of  65  dogs  weighed  ami  experimented  on  by  Chlopin  the  average 

weigh!  waa  ,.».•-,  kilograms,  or  20.3  pound.-:  almost  half  the  d 
weighed  between  <">  ami  11  kilos. 

To  adapt  the  rules  of  Leliiiinnu  to  a  basis  of  grains  per  100  poundsof 
body  weight,  assuming  the  average  weight  of  a  dog  to  be  20  pounds, 


158         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

it  is  only  necessary  to  multiply  the  weight  of  color  by  5  and  by 
15.432.     Doing  so,  the  following  data  are  obtained: 

A.  Harmful  colors  produce  bad  e  fects  in  doses  of  a  "few"  decigrams,  i.  e.,  mul- 
tiples of  a  half  gram;  the  word  "few"  is  not  sharply  denned,  but  the  rule  means  a 
"few"  times  7.7  grains. 

B.  Harmless  colors  produce,  when  continuously  fed,  no  bad  effect  in  multiples  of 
10  of  the  doses  of  A,  above,  i.  e.,  multiples  of  77  grains. 

I  Slight  diarrhea  and  slight,  temporary  albuminuria  are  not  to  count  against  the 
color. 

Applying  these  rules  to  the  preceding  colors  discloses  that  they  were 
apparently  not  so  used,  in  selecting  the  harmless  and  harmful  colors 
in  the  Confectioners'  List. 

LEHMANN'S  RULES. 

The  Lehmann  rules  as  just  interpreted  were  applied  to  the  data 
just  given.  As  a  result  of  such  application  the  conclusion  is  reached 
that  of  the  15  colors  classed  as  harmless  (foregoing  classes  I,  II,  and 
III),  6  would  be  classed  as  doubtful  by  the  Lehmann  rules,  namely: 

13.  Ponceau  4  GB,  65.  Fast  Red  B, 

8  and  9.  Fast  Yellow  Y  and  R,  103.  Azorubin  S, 

55.  Ponceau  2R,  105.  Fast  Red  E, 

and  the  remaining  9  would  have  been  classed  as  harmless. 

Of  the  11  classed  as  harmful  (foregoing  classes  I,  II,  III,  and  IV), 

2  would  have  been  regarded  as  harmless,  namely: 

308.  Xaphthol  Green  B,  138.  Fast  Brown  (1, 

3  would  have  been  classed  as  doubtful,  namely: 

197.  Bismarck  Brown,  88.  Diphenylamin  Orange, 

11.  Sudan  I, 

and  the  remaining  6  would  have  been  classed  as  harmful. 
SANTORI'S  WORK  AS  A  GUIDE  TO  A  RULE. 

Santori  regards  the  following  six  dyes  as  harmless:  157  (18S), 
467  (74),  477  (129.5),  4S0  (156),  599  (64),  092  (467). 

The  first  is  the  Green  Table  number  and  the  bracketed  figure  the 
average  Dumber  of  grains  per  100  pounds  per  day  for  30  days. 

In  the  case  of  Nbs.  457  and  599  the  animal  was  wholly  normal 
throughout  the  test  and  the  autopsy  showed  only  normal  conditions. 

In  the  case  of  \o.  477  (he  only  disturbance  w  is  colored  feces  and 
the  autopsy  showed  only  normal  conditions. 

In  tin1  case  of  No.    ISO  the  only  disturbance  was  colored  feces,  but. 

the  autopsy  showed  a  pea-green  kidney. 

In  the  case  of  Nbs.  167  and  692  there  was  only  vomiting;  in  the 
of  N<>.  167  the  autopsy  showed  everything  normal;  whereas  in  the 
of  No.  692  the  autopsy  disclosed  a  swollen  kidney. 

Therefore,   according  to  Santori,   a  dyv   that  causes  colored    feces, 

even  with  colored  kidney,  is  harmless.     Also  a  dye  that  causes  vomit- 


OIL-SOLUBLE   OK  TAT   COLORS.  159 

ing  and  swollen  kidney  is  harmless.  On  the  other  hand,  a  dye  (572) 
which  produces  no  change  or  symptom  observable  during  life,  but 
fatty  degeneration  of  the  liver  is  shown,  at  the  autopsy,  is  a  harmful 
dye.  This  lack  of  conformity  makes  the  relation  between  dosage, 
symptoms,  and  harmfulness  or  harmlessness  more  confusing  and  per- 
plexing. 

YOUNG'S  RULE. 

It  must  be  remembered  that  smaller  amounts  of  drugs,  and,  there- 
fore, of  coal  tar  colors,  effect  children  as  a  rule  than  are  effective 
upon  adults.  Taking  Young's  rule  as  a  guide,  it  appears  that  gen- 
erally the  effective  dose  for  a  3-year-old  child  is  one-fifth  the  effec- 
tive adult  dose;  for  a  4-year-old  child  one-fourth;  for  a  6-year-old 
child  one-third;  for  an  8-year-old  child  two-fifths  and  for  a  12-year- 
old  child  one-half  the  effective  adult  dose.  All  of  this  should  be  taken 
into  account  in  drawing  conclusions  from  experiments  as  to  the  harm- 
lessness of  any  coal-tar  dye  upon  humans.  Very  little  attention  has, 
however,  been  paid  to  this  aspect  of  the  matter  in  spite  of  the  fact 
that  colored  foods,  confectionery,  pastry,  beverages,  and  the  like  are 
partaken  of  by  children  and  in  many  cases  such  articles  are  prepared 
for  the  sole  or  particular  consumption  of  the  very  young. 

From  the  foregoing  data  it  seems  clear  that  deductions  as  to  the 
harmlessness  or  harmfulness  of  coal-tar  dyes  when  administered  to 
dogs,  and  not  based  upon  autopsies,  are  not  final  nor  conclusive  as  to 
the  effect  upon  the  dog.  The  extent  to  which  such  deductions  are 
correctly  transferable  to  humans  is  likewise  not  established. 

XI.  OIL-SOLUBLE  OR  FAT  COLORS. 

Oil-soluble  colors  are  used  for  coloring  fats,  such  as  butter,  oleo- 
margarine, edible  oils,  and  the  like;  of  the  coal-tar  colors  the  oil- 
soluble  colors  are  chemically  nonsulphonated  azo-colors. 

The  nonsulphonated  azo-colors  which  have  been  physiologically 
examined  arc: 

11.  Sudan  1  (anilinaxo-b-naphthol)  ('J*. 

Hi.  Butter  Yellow  (anilin-aso-dimethylanilin). 

17.  Chrysoidin  V  (anilin-aso-m -phen}  lene-diamin 

18.  ChryBoidin  R  (aniliiia&o-m-tolylene-diamin)  (1). 
11.  ChryBoidio  R  (o-toluidin-aso-m-tolylene-diamin). 

li)7.  Bismarck  Brown  (m-phenylene^iajum-disftzo-m-phenylene^iamix)     I 
201.  Manchester  Brown  (m  tolj  lene-oUamin^isaxo-m-tolylene-diamin 

The  numbers  preceding  the  trade  Dames  arc  the  Green  Table  num- 
bers; ili'1  scientific  aames  appear  in  parentheses;  and  the  number  of 
dealers  offering  the  colors  on  the  United  States  market  in  the  summer 
of  1907,  out  of  a  possible  12,  appear  after  the  scientific  name,  also  in 
parentheses. 


160         COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

For  all  but  No.  201  contradictory  statements  occur  in  the  compiled 
literature;  for  Xo.  201  only  unfavorable  reports  were  found. 

There  were  on  the  United  States  market  in  the  summer  of  1907  the 
following  oil-soluble  colors: 

10.  Sudan  G  (anilin-azo-resorcin)  (1). 

11.  Sudan  I  (anilin-azo-b-naphthol)  (2). 

4U.  Sudan   II   (xylidin-azo-b-naphthol)   (1). 

60.  Carminaph  Garnet  (a-naphthylamin-azo-b-naphthol)  (1). 

<  these  No.  11  had  been  reported  on  contradictorily,  and  the 
remaining  three  had  not  been  reported  on  at  all.  In  addition  to  these 
the  following  three  oil-soluble  colors,  not  listed  m  the  Green  Tables 
and  not  reported  on  in  literature,  were  wanted: 

1.  o-Toluidin-azo-b-naphthylamin  (which  does  not  seem  to  be  described  in  litera- 
ture in  any  way). 

2.  Amidoazo-toluol. 

3.  Anilin-azo-b-naphthylainin. 

So  that  out  of  a  total  of  seven  oil-soluble  colors  on  the  United 
States  market  in  the  summer  of  1907  only  one  had  been  examined 
physiologically  and  that  with  contradictory  results.  As  before 
stated,  these  oil-soluble  colors  all  belong  to  the  class  of  nonsulpho- 
nated  azo-colors. 

Fraenkel  (p.  575)  says:  "When,  however,  the  azo-colors  contain 
no  sulpho-group  (i.  o.,  are  nonsulphonated)  they  are  poisonous. 
Thus  for  example,  Bismarck  Brown  *  *  *  Sudan  I."  Yet 
meta-nitrazotin,  a  nonsulphonated  color  not  in  the  Green  Tables, 
and  probably  not  upon  the  market  anywhere,  and  which  is  meta- 
nitranilin-azo-b-naphthol,  is  according  to  Weyl  nonpoisonons. 
Fraenkel  (p.  575)  also  stated: 

The  fact  that  the  monazo  colors  examined  by  Cazeneuve  and  Lepine  arc  harmless, 
a?  above  stated,  is  equally  explained  by  the  constitution  ot*  these  substances.  Those 
two  investigators  examined  (omitting  the  trade  names)  a-naphthylamin-sulphoacid- 
a/.o-a-naphthol-a-sulphoacid,  a-naphthylainin-sulphoacid-a/.o-  b-  naphthol  -disulpho- 
acid,  a-naphthylamin-azo-b-naphthol-disulphoacid,  xylitlin-a/.o-b-naphthol-disulpho- 
acid,  Milphaiiilicarid-azo-a-naphtho],  Amido-a-zo-toluene-disulphonicacid. 

These  substances  arc  all  sulphoacids  and  the  sulpho-groupe  here  effect  the  d<'i>oi8on- 
ing  of  the  original  substance. 

Examining  this  statement  it  therefore  appears  that  in  Fraenkel's 
opinion,  at  least,  a-naphthylamin-azo-a-naphtihol,  a-naphthylamin- 
azo-b-naphthol,   xylidin-azo-b-naphthol,   anilin-azo-a-naphthol,   and 

amido-azo-toluol  are  in  and  of  themselves  poisonous  substances,  and 
arc  rendered  nonpoisonons  by  snlphonation.  Diligent  search  through 
the  literature  has  failed  to  uncover  any  original  communications  of 
investigators  to  that  effect. 

With  hut  one  known  exception  all  the  nonsulphonated  azo-colors 

egarded  by  Fraenkel  as  poisonous.  The  colon  17,  IS,  41,  197, 
and  201  on  page  159  are  not  used  as  oil-soluble  colors  and  therefore 
form  no  comparative  basis  for  judging  oil-eoluble  colors  exeept  that 


REASONS    FOR   SELECTING   SEVEN   PERMITTED   COLORS.  161 

both  are  nonsulphonated  azo-colors;  in  FraenkeFs  opinion,  however, 
such  a  comparison  is  wholly  justified  and  proper. 

Excluding  now  17,  18,  41,  197,  and  201  for  the  purposes  of  com- 
parison, the  following  tabulation  is  made: 

Oil-soluble  nonsulphonated  azo-colors  on  the  market,  1907,  deemed  poisonous  by  Fraenhel. 


Oil-soluble  colors.  States  calls 

market.      poisonous. 


anilin-azo-resorcin x  

anilin-azo-b-naphthol x  x 

xyii<lin-azo-b-naphthol x  x 

a-naphthylamin-azo-b-naphthol :  x  x 

o-toluidin-azo-b-naphthylamin i  x  

araido-azo-toluol x  x 

anilin-azo-b-naphthylamin x  

a-naphthylamin-azo-a-naphthol x 

anilin-azo-a-naphthol x 

That  is,  the  only  ones  on  the  United  States  market  concerning 
which  no  expression  of  specific  opinion  is  to  be  found  in  Fraenkel  are 
the  following  three:  anilin-azo-resorcin,  toluidin-azo-b-naphthylamin, 
and  anilin-azo-b-naphthylamin,  and  notliing  is  published  on  the 
physiological  action  of  any  of  them  specifically.  The  probability, 
however,  would  seem  to  be  that  they  are  not  harmless,  and  until 
their  harmlessness  is  positively  established  their  exclusion  from  the 
permitted  list  of  coal-tar  colors  for  use  in  foods  seems  to  be  the  only 
safe  and  proper  course  to  be  followed.  The  physiological  action  of 
so-called  "Butter  Yellow"  No.  16  of  the  Green  Tables  (see  p.  85), 
merely  strengthens  tins  conclusion. 

XII.   RULES  AND  REASONS  FOR  SELECTING  THE  SEVEN  COLORS 
PERMITTED  BY  F.  I.  D.  76. 

STATEMENT  OF  RULES. 

In  view  of  the  confusion  and  uncertainly  disclosed  in  the  foregoing 
literature  relative  to  the  physiological  action  of  coal-tar  colors,  the 
difficulties  in  the  way  of  making  a  list  of  coal-tar  colors  to  be 
permitted  in  the  coloring  of  food  products  are  seen  to  be  by  ao 
means  slight .  The  following  rules  governing  selection  were  in  mind 
fining  the  making  of  the  list  given  in  Food  [nspectioo  Decision  No.  76, 
and  the  closeness  with  which  they  were  followed  is  discussed  on 
L66. 

Rule  [.  All  colors  which  have  not  been  physiologically  tested  either 
upon  animals  or  man  shall  not  he  permitted  for  use  in  foods. 

Knlell.  All  COal-tar  Colors  which  have  been  examined  physio- 
logically with  contradictory  results  shall  not    he  permitted  for  U8S  in 

ft  "  mIs. 

>1°— Bull.  J  i:     u    —11 


162 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Rule  III.  All  coal-tar  colors  which  have  been  examined  physiologi- 
cally and  have  been  declared  to  be  of  doubtful  harmlessness  shall  not 
be  permitted  for  use  in  foods. 

Rule  IV.  Only  those  coal-tar  colors  whose  chemical  composition 
was  definitely  disclosed  or  otherwise  ascertained,  and  winch  were  on 
the  United  States  market  in  the  summer  of  1907,  and  winch  have 
been  examined  physiologically  and  with  no  other  than  a  favorable 
result  shall,  for  the  present,  be  permitted  for  use  in  foods. 

ANALYSIS  OF  THREE  RECOMMENDATIONS  MADE  TO  THE  DEPART- 
MENT OF  AGRICULTURE. 

These  rules  were  formulated  as  a  guide  in  view  of  the  divergent 
opinions  expressed  in  three  different  recommendations  to  the  Depart- 
ment of  Agriculture.  One  of  these  recommendations  suggested  that 
permitted  colors  be  designated  by  nine  titles.  Comparison  of  these 
titles  with  the  Green  Tables  and  with  the  tabulated  survey  of  the  unfa- 
vorable, favorable,  and  contradictory  literature  corresponding  to  the 
Green  Table  numbers  (p.  63)  discloses  the  following  facts: 

Comparison  of  nine  suggested  color  titles  with  corresponding  Green  Table  numbers  and 

the  reports  on  the  same. 


Name. 

Green 

Table 

No. 

Un- 
favor- 
able. 

Fa- 
vor- 
able. 

Con- 
tra- 
dic- 

tory. 

No 
re- 
port.1 

Name. 

Green 

Table 
No. 

Un- 
favor- 
able. 

Fa- 
vor- 
able. 

Con- 
tra- 
dic- 
tory. 

No 
re- 
port.1 

Chrysoidin 

17 
18 
41 
84 
85 
86 
87 
88 
95 
92 
102 
13 
15 
44 
55 
56 
57 
108 
114 
140 

X 
X 
X 
X 

Ponceau  

147 
148 
150 
1()0 
163 
169 

65 
107 
157 
170 
171 
198 
244 

M 

46a 

1 

X 

Tropueolin 

X 
X 

X 

X 
X 
X 
X 

X 
X 
X 

Blebrich  Red  (?).. 
8  ii  l  p  b  o  d  a  t  e  d 

X 

X 
X 

X 

X 

X 
X 

X 

X 
X 
X 
X 
X 

X 

X 
X 

Naphlhol    Yellow 
S 

Total 

36 

0 

8 

13 

15 

1  Of  physiological  tests  in  literal  lire  Compiled. 

Therefore,  under  9  titles  36  di  Ferenl  chemical  individuals  would 
be  placed  upon  i  lie  permitted  list ,  of  which  only  8,  or  less  i  ban  25  per 
cent,  bave  been  examined  physiologically  with  only  favorable 
results,  and  28,  ot  more  I  ban  75  per  cent ,  had  either  not  been  examined 
at  all  physiologically  or  with  contradictory  results. 


REASONS  FOR  SELECTING  SEVEN  PEEMITTED  COLORS. 


163 


The  8  of  these  chemical  individuals  examined  xvith  only  favorable 
results,  and  the  number  of  sources  out  of  a  possible  12  offering  them 
on  the  United  States  market  in  the  summer  of  1907,  are  as  follows: 

Colon  reported  on  favorably  and  number  of  dealers  handling  same. 


Green 

Table 

No. 

Sources 
offering. 

Green 

Table 

No. 

Sources 
offering. 

M 
65 
86 

92 

10 
2 

2 
0 

102 
107 
169 
462 

0 

i 

2 

1  The  italicized  Green  Table  numbers  are  those  of  the  permitted  list  of  Food  Inspection  Decision  No.  76. 

Another  recommendation  suggested  the  permissive  use  of  42 
entries  in  the  Green  Tables,  which  are  tabulated  below  in  the  same 
manner  as  the  suggestions  in  the  preceding  recommendation: 

Comparison  of  42  recommended  Green  Table  numbers  with  reports  in  the  literature. 


Green 
table 
No. 

Un- 
favor- 
able. 

Favor- 
able. 

Equiv- 
ocal. 

No 
report.1 

Green 
table 
No. 

Un- 
favor- 
able. 

Favor- '  Equiv- 
able.       ocal. 

No 
report.1 

4 
8 
17 
50 
53 
54 
55 
65 
85 
86 
89 
92 
94 
LOT 
103 
107 
138 

tea 

166 

l's7 

X 

427 
434 
44s 
451 
456 
457 
462 
477 
478 
479 
480 
504 
512 
513 
514 
516 
517 
5is 
50'2 
601 

Total 

X 

X 
X 

' 

x       | 
X 

X 

X 

X 

X 

X 

X 

X 
X 

X 
X 

X 

X 

X 

X 

X 
X 

X 
X 

X 

X 
X 
X 

X 
X 

X 

X 
X 

X 

X 
X 

X 
X 

X 

X 
X 

5 

14 

15 

8 

1  Of  phyriologtoal      I    In  compiled  literature. 

Applying  the  conclusions  hereinbefore  reached  i<>  these  entries, 
it  is  found  that    1  !  out  of  the  42  colors  recommended,  or  exactly 

One-third,   had    been   examined    physiologically    with   only    favorable 

results,  and   the   remaining  two-thirds  had   been   either  examined 

physiologically    with    only    unfavorable    of-    with    conflicting    results, 

d  not  been  examined  at  all. 

Hie   M   chemical  individuals  examined   with   favorable  result  and 
tin'   number   of   BOUrcee   OUl    of   a    possible    \2   offering    them    on    the 

United  State-  market  in  the  summer  of  1907  are  a-  follows: 


164         COAL-TAB  COLORS  USED  IN  FOOD  PRODUCTS. 

Colors  reported  on  favorably  and  number  of  dealers  handling  same. 


Green 
table 
No. 

Sources 
offering. 

Green 
table 
No. 

Sources 
oifering. 

U 
65 
85 
89 
92 
102 
103 

10 
2 
2 
1 
0 
0 
6 

107 
166 
240 
462 
477 
512 
577 

0 
1 
2 
0 
3 
E 

*  The  italicized  Green  Table  numbers  are  those  of  the  permitted  list  of  Food  Inspection  Decision  No.  76. 

The  third  of  these  recommendations  suggested  27  different  chemical 
individuals  for  permissive  use;  these  are  tabulated  below  in  the  same 
manner  as  the  suggestions  in  the  preceding  recommendations. 

Twenty-seven  colors  recommended  for  use  and  reports  in  the  literature  on  the  same. 


Green 
table 
No. 

Un- 
favor- 
able. 

Favor- 
able. 

Equiv- 
ocal. 

No 
report.1 

Grern 
table 
No. 

Un- 
favor- 
able. 

Favor- 
able. 

Equiv- 
ocal. 

No 
reports 

4 

16 

17 

18 

41 

65 

85 

102 

197 

201 

398 

457 

462 

476 

477 

X 

481 
512 
516 
517 
518 
521 
532 
584 
601 
602 
650 
692 

Total 

X 

X 
X 
X 
X 

X 

X 

X 

X 

X 

X 
X 

X 

X 

X 
X 

X 

X 

X 

X 
X 

X 

X 

X 

X 

4 

10 

10 

3 

X 

1  Of  physiological  tests  in  literature  compiled. 

Therefore,  applying  the  same  method  of  drawing  conclusions  as 
in  the  case  of  the  preceding  two  recommendations,  it  appears  that 
10  out  of  the  27  suggested  chemical  individuals  had  been  examined 
physiologically  with  only  favorable  results,  and  the  remaining  17 
had  either  not  been  examined  at  all  or  with  unfavorable  or  con- 
flicting results.  The  10  chemical  individuals  examined  with  favorable 
results,  and  the  number  of  sources  out  of  a  possible  12  offering  them 
on  the  United  States  market  in  tho  summer  of  1907,  are  as  follows: 

The  10  recommended  colors  favorably  reported  on  in  the  literal  are  and  the  dealers  handling 

same. 


Green 

Bouroei 

Green 

Souroea 

Table 

han- 

Table 

han- 

No. 

dling. 

No. 

dling. 

W 

id 

•177 

0 

2 

6i  a 

8 

M 

2 

r,n 

6 

KIJ 

0 

:,'i 

0 

462 

2 

692 

3 

*Tho  italicized  Ghm-ii  Table  Qtimbexi  in  thoie  tA  the  permitted  list  of  Food  Inspection  Decision  No.  76. 


REASONS  FOR  SELECTING  SEVEN  PERMITTED  COLORS. 


165 


All  of  the  colors  included  in  these  three  recommendations  con- 
cerning which  only  favorable  reports  were  found  in  the  literature  are 
given  in  the  following  table : 

Recommended  colors  favorably  reported  on  in  the  literature. 


Recommendations. 

Recommendations. 

Green 

Dealers 

Green 

Dealers 

Table 

otter- 

Table 

offer- 

No. 

I. 

ir.     in. 

Total. 

ing. 

No. 

I. 

ii. 

III. 

Total. 

ing. 

U 

X 

X              X 

3 

10 

240 

X 

1 

1 

65 

X 

X 

X 

3 

2 

462 

X 

X 

X 

3 

2 

85 

X 

X 

X 

3 

2 

477 

X 

X 

2 

0 

89 

X 

1 

1 

512 

X 

X 

2 

3 

92 

X 

X 

2 

0 

617 

X 

X 

2 

5 

102 

X 

X 

X 

3 

0 

521 

X 

1 

0 

103 

X 

1 

8 

692 

X 

1 

3 

U07 
166 
169 

2 

1 
1 

7 
0 

1 

X 

X 

Total  . 

8 

14 

10 

i  The  italicized  Green  Table  numbers  are  those  of  the  permitted  list  of  Food  Inspection  Decision  No.  76. 

This  table  is  now  rearranged  to  show — 
I.   The  recommended  colors  not  offered  in  the  United  States  market  in  the  summer  of  1907. 


Green 

Table  No. 

Recom- 
mended 

by- 

Green 
Table  No. 

Recom- 
mended 

by- 

92 
102 
166 

2 
3 

1 

477 
521 

2 

1 

II.    The  recommended  colors  offered  on  the  United  States  market  in  the  summer  of  1907. 


Green 
Table  No. 

Recom- 
mended 

by- 

Sources 
handling. 

Green 
Table  No. 

Recom- 
mended 
by- 

Sources 
handling. 

M 
65 
86 
89 
103 
107 

3 
3 
3 

1 
1 
2 

10 
2 
2 

1 

168 

240 

612 

617 
692 

l 
1 
3 
2 
2 

1 
1 
2 
3 
5 
3 

i  The  italicized  Green  Table  numbers  an-  those  of  the  permitted  list  of  Food  Inspection  Decision  No.  76- 

It  appears  that  out  of  17  different  chemical  individuals  suggested 
by  these  3  recommendations  jointly,  5  were  not  on  the  United  Statei 
market  in  the  summer  of  L  907,  and  L2  were  on  thai  market;  also  that 
of  these  12,  4  were  suggested  by  all  :;  recommendations;  3  were 

wanted  by  only  2  out   of  llie  .!.    and  the  remaining  5  were  spoken  for 

by  only  one.     Examining  all  of  the  recommendations,  it.  appears 
that.  out.  of  a  total  of  79  recommendations  1 7  bad  been  examined  with 

only  favorable   results,    and    that    the   remaining  62   were  either   not 

examined  or  had  been  examined  with  unfavorable  or  conflicting 

results. 

To  add  to  the  confusion  the  third  recommendation  mentioned  sug- 
gested that  the  following  ( oven  Table  numbers  should  not  f>e  permit- 


166         COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

ted  for  use  in  food  products  because  they  are  harmful :  1 ;  2 ;  3 ;  6 ;  86 ; 
95;  425;  451;  454;  480;  483;  484;  487;  488;  490;  571;  584;  599; 
620;  624;  650.  The  same  paper,  however,  recommended  that  Nos, 
584  and  650  be  permitted  for  use  in  food  products;  that  No.  86,  sug- 
gested by  both  the  other  recommendations,  be  prohibited;  and  that 
Nos.  95,  451,  and  480,  suggested  by  one  or  the  other  of  the  remaining 
two  recommendations,  be  likewise  prohibited  for  use  in  food  products. 
It  must  be  clear  to  everyone  that  these  three  recommendations  are 
not  of  one  mind  as  to  (1)  the  colors  which  are  harmless;  (2)  the 
colors  which  are  harmful;  (3)  vho  colors  which  are  used  or  are  useful 
in  food  coloring;  and  (4)  the  colors  which  should  be  used  in  food 
coloring.  Such  a  state  of  affairs  fully  justifies  rules  of  the  scope  and 
intent  of  those  formulated  at  the  beginning  of  this  section  for  making 
a  selection  of  permissible  food  colors. 

PROCESS  OF  ELIMINATION. 

From  the  foregoing  data  it  appears  that  out  of  80  different  chemical 
individuals  on  the  food-color  market  of  the  United  States  in  1907, 
only  16  had  been  examined  physiologically  with  a  favorable  result 
(see  p.  64). 

These  16,  arranged  according  to  the  shade  produced,  are  as  follows 
(numbers  preceding  the  names  are  the  Green  Table  numbers;  the 
numbers  in  parentheses  show  the  number  of  sources  desiring  the  color; 
the  italicized  Green  Table  numbers  are  the  ones  finally  selected  by 
Food  Inspection  Decision  No.  76) : 


65.  Fast  Red  B  (Alphanaphthylamin  azo-R-salt)  (2). 
103.  Azorubin  S  (Naphthionic  acid  azo  NW  acid)  (6). 
105.  Fast  Red  E  (Naphthionic  acid  azo-Schaeffer  acid)  (1). 
107.  Amaranth  (Naphthionic  acid  azo-R-salt)  (7). 

169.  Crocein  Scarlet  713  (Amidoazotolutol-monosulphonic-acid-azo-betanaphthol- 
monosulphonic  acid  B)  (1). 
240.  Congo  Red  (Benzidin  di.sazo-naphthionic  acid)  (1). 
4G2.  Acid  Magenta  (Magenta  trisulphonic  acid)  (2). 
512.  Eosin  A  (Tetra-bromo-fluorescein)  (3). 
517.  Erythrosin  (Tetra-iodo-flnorcBcein)  (5). 
520.  Rose  Bengal  (Dichlor-tetraiodo-fluorescein)  (2). 

ORANGE. 

85.  Orange  I  (Sulphanilic  arid  azo-alpha-naphthol)  (2). 

FELLOWS. 

4.  Naphthol Yellow (DinitroalphanaphtholBulpho  acid)  (10). 
89.  Brilliant  Yellow  S  (Sulphanilic  acid  azo-diphcnylaniin,  sulphonated)  (1). 

433.  Guinea  Green  B  (Benzyldehyde  +  benzylethyanilin  Bulpho-acid)  (1). 

..  Light  Green  8   F  yellowish  (Beniyldehyde+benxylethylanilin-fiulphona- 
tton)  (4). 


REASONS  FOR  SELECTING  SEVEN  PERMITTED  COLORS.     167 

BLUE. 

692.  Indigo  Carmine  (Indigo  disulpho  acid)  (3). 

Considering  now  the  reds,  and  particularly  107,  which,  as  the  num- 
ber appearing  in  parentheses  after  the  scientific  name  indicates,  was 
wanted  by  7  sources  out  of  the  12  drawn  on,  this  being  the  most 
desired  of  all  the  reds,  it  would  seem  reasonable  to  believe  that  all  the 
wants  supplied  by  65,  103,  105,  169,  240,  and  462  would  be  covered 
by  107.  Chemically  107  is  closely  allied  to  65,  103,  105,  and  tinc- 
torially it  is  likewise  closely  allied  to  169,  240,  and  462. 

Nos.  512,  517,  and  520  are  chemically  quite  different  from  the  other 
members  of  this  group,  and  tinctorially  they  differ,  being  of  a  particu- 
larly brilliant  shade,  and  tinctorially  more  powerful;  517  being 
desired  by  5  out  of  the  12  sources  drawn  upon,  and  thus  being  the 
most  desired  of  these  three  colors,  was  selected  in  the  expectation 
that  any  work  512  and  520  could  do  in  food  products  would  be  equally 
well  done  by  517.  For  reds,  therefore,  the  choice  fell  upon  107  and 
517. 

Orange. — Only  one  color  was  wanted,  and  that  by  2  out  of  the  1 2 
sources,  and  this  was  placed  in  the  permitted  list. 

Yellows. — The  choice  of  No.  4,  which  was  wanted  by  10  out  of  the 
12  sources,  was  made  in  the  expectation  that  every  purpose  that  89 
could  serve  in  food  products  could  be  served  also  by  4. 

Greens. — Tinctorially  and  chemically  the  two  greens  are  very 
closely  allied,  and  in  view  of  the  reasonableness  of  the  expectation 
that  435  could  do  all  the  work  of  433  as  well,  its  choice  was  regarded 
as  justified,  especially  as  435  was  wanted  by  4  out  of  the  12  sources, 
as  against  only  one  for  433. 

Blue. — Xo.  692  being  regarded  as  harmless  by  all,  and  being  the 
only  blue  in  the  list,  it  was  selected. 

In  this  manner  six  out  of  the  seven  permitted  colore  were  selected. 

REASONS  FOR  ADDING  PONCEAU  3R. 

An  examination  of  the  table  on  page  20  discloses  the  fact  that 
among  the  reds  desired  four  were  azo-reds  made  from  anilin  deriva- 
tives as  the  first  component,  namely: 

53.  Xylidin-azo-alj>lmn:i|>hth<>l<lisulpho  acid. 

54.  Xylidin-azo-Schaeffer  acid. 

55.  Xyli<lin-nzo-ll-~ali . 

56.  Cumidin  aso-R-eal! . 

Kaeh  of  these  was  wanted  by  1  source  out  of  the  possible  12.      This 

was  construed  as  an  expression  of  a  real  Deed  in  the  ait  of  food  coloring 

for  a  color  of  this  class.     The  reason  forsuch  a  need  was  n<>t.  then,  nor 

is  it  now,  apparent,  but  the  propriety  of  giving  even  a  seeming  need 

due  consideration  w  as  regarded  as  justified.      For  only  one  of  the  four 
desired, namelj,  55,  could  any  speciiic  references  in  the  literature  be 


168        COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

found,  and,  in  fact,  four  references  were  found  favorable  thereto  and 
three  unfavorable  thereto;  thus  eliminating  55  from  consideration, 
leaving  53,  54,  and  56. 

The  Austrian  law  of  January  22,  1896  (see  Lieber,  p.  15),  permits 
the  use  of  azo  colors  derived  from  higher  homologues  of  anilins, 
beginning  with  xylidin  and  sulphonated  betanaphthols.  As  Nos.  53 
and  54  were  both  derived  from  xylidin,  it  was  regarded  as  safe  to 
assume  that  they  would  probably  be  as  objectionable  as  55.  This 
left  56  only  to  be  considered,  which  color  is  derived  from  cumidin 
and  R-salt.  The  cumidin  portion  satisfies  the  Austrian  law  and  also 
satisfies  the  general  law  laid  down  in  Fraenkel  (p.  162),  namely,  that 
the  greater  the  number  of  ring-methyls  the  less  the  toxic  property  of 
the  resulting  compound,  because  of  the  oxidation  of  these  methyls  to 
carboxyls  in  the  animal  system;  the  R-salt  portion  satisfies  the  gen- 
eral law  laid  down  in  Fraenkel,  that  the  more  highly  sulphonated  the 
less  toxic  a  substance  becomes,  and  therefore  56  is  in  the  first  portion 
of  its  composition  of  such  a  nature  as  to  be  less  objectionable  than  55, 
if  55  be  objectionable. 

This  combination  of  facts,  namely,  the  desirability  of  an  anilin 
azo-red,  the  provision  for  diminishing  the  toxicity  of  55  by  the  sub- 
stitution of  cumidin  for  xylidin  therein,  and  the  general  provision 
in  the  Austrian  food  law,  made  it  appear  desirable  and  safe  to  take 
into  account  an  anilin  azo-red,  and  therefore  to  select  56  as  probably 
the  least  objectionable,  if  it  be  at  all  objectionable,  of  the  anilin 
azo-reds. 

The  full  list  of  permitted  colors  was  therefore  extended  to  7,  as 
follows : 

Red  shades. — 107.  Amaranth;  56.  Ponceau  3R;  517.  Erythrosin. 

Orange  shade. — 85.  Orange  I. 

Yellow  shade. — 4.  Naphthol  Yellow  S. 

Green  shade. — 435.  Light  Green  S  F  yellowish. 

Blue  shade. — 692.  Indigo  disulpho  acid. 

It  should  be  noted  that  with  respect  to  tetra-iodo-fluorescein,  517 
of  the  Green  Tables,  no  specific  investigation,  pronouncing  it  harmless 
or  harmful,  is  described  in  the  literature.  No.  516,  the  diodo-fluores- 
cein,  is  reported  specifically  adversely  in  the  literature,  especially  by 
Chlopin;  the  Confectioners'  List,  the  laws  of  Austria,  the  lawrs  of 
France,  the  rather  superficial  examination  of  No.  517  by  Gran dho mine, 
and  the  statement  in  Fraenkel  (p.  574)  >  that  it  produces  no  disturbance, 
are  all  taken  to  apply  to  517  and  not  to  516.  The  identification  of  the 
color  under  examination  with  517  has  not  in  all  cases  been  satisfac- 
torily exclusive,  but  it  is  believed  that  the  differentiation  of  the 
harmful  516  by  Chlopin  makes  all  the  other  references  cited  pertinent 
to  517. 


LISTS   OF   COLORS   RECOMMENDED  BY  INDIVIDUALS.  169 

With  respect  to  435,  it  must  be  pointed  out  that  434,  which  is  the 
methyl  instead  of  the  ethyl  derivative,  has  only  been  regarded  as 
suspicious,  and  one  examination  of  435,  namely,  that  of  Lieber 
(p.  144),  does  not  appear  to  disclose  anything  which  would  positively 
exclude  435. 

QUALITY,  CLEANLINESS,  AND  EFFICIENCY. 

The  justification  for  limiting  the  permitted  colors  to  6  out  of  16, 
against  which  nothing  unfavorable  is  contained  in  the  literature  and 
regarding  which  favorable  statements  are  at  hand,  and  the  addition 
to  these  6  of  the  seventh  color  is  to  be  found  in  the  very  great  variation 
in  tinctorial  quality,  in  percentage  of  coloring  matter,  in  amounts 
of  insoluble  matter,  both  organic  and  inorganic,  and  in  the  amounts 
of  organic  matter  not  coloring  matter,  as  well  as  in  the  large  number 
of  samples  containing  an  amount  of  arsenic  in  excess  of  that  permitted 
by  the  United  States  Pharmacopoeia  for  the  only  coal-tar  color 
therein  mentioned,  namely,  Methylene  Blue,  and  the  varying  amounts 
of  heavy  metals,  such  as  copper,  lead,  and  iron,  mostly  in  excess  of 
the  limits  permitted  in  the  Pharmacopoeia  for  various  medicinal 
chemicals.  This  wide  variation  in  quality  and  degree  of  cleanliness, 
all  pointing  to  a  very  great  difference  in  the  care  with  which  coal-tar 
colors  offered  for  food  purposes  are  prepared,  render  the  conclusion 
safe  that  some  control  over  food  colors  in  respect  to  quality  is  desir- 
able, necessary,  and  essential. 

The  efficiency  of  the  7  colors,  6  of  winch  were  selected  from  among 
the  16  considered  for  the  purpose  of  making  this  list  of  permitted  colors 
as  being  reasonably  sure  to  be  harmless,  is  evidenced  by  the  fact  that, 
although  the  addition  of  colors  has  been  sought  by  persons  interested 
in  the  food-coloring  art,  not  one  of  the  remaining  10  colors  of  those 
16  has  been  so  requested.  In  other  words,  the  colors  that  the  depart- 
ment has  boon  requested  to  add  to  the  permitted  list  were  outside 
of  the  16  colors  which  were  on  the  markets  of  the  United  States  in 
1907,  and  were  described  in  the  literature  in  such  a  manner  as  to  lead 
to  the  conclusion  that  they  were  probably  not  harmful. 

XIII.  LISTS  OF  COLORS  SUBSEQUENTLY  RECOMMENDED  BY 
INDIVIDUALS  AND  ASSOCIATIONS. 

Since  Food  Inspection  Decisions  Nos.  7(>  and  77  were  published 
recommendations  of  lists  of  permitted  colors  have  been  made  by 
other  individuals  and  by  a  voluntary  association.  For  the  purpose 
of  comparing  these  proposed  lists  of  permissible  colors  with  the  per- 
mitted list  of  Pood  [nspection  Decision  No.  76,  the  former  are  now 
to  be  examined  in  (he  same  manner  as  the  coal-tar  colors,  on  the 
United  States  market  in  the  Bummer  of  1907  for  food  coloring  pur- 


170 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


poses,  were  examined  in  order  to  establish  the  permitted  list  of  7 
colors.     These  recommendations  cover  the  following  lists: 

1.  W.  Ernst's  list. 

2.  Muttelet's  interpretation  of  the  French  law. 

3.  Second  International  White  Cross  Congress  list. 

4.  Beythien  and  Hempel's  list. 

5.  An  American  manufacturer's  list. 

6.  Belial's  list. 


ERNST. 

W.  Ernst  (Fdrber  Zeitung  1908,  vol.  19,  p.  381;  abst.  CTiem.  Ztg. 
u  Reportorium"  1909,  p.  89)  recommends  for  use  in  foods  the  following 
38  titles  of  coal-tar  colors.  The  Green  Table  numbers  appear  in 
parentheses  after  each  title  where  corresponding  numbers  could  be 
ascertained;  the  italicized  numbers  are  those  of  the  permitted  list 
of  Food  Inspection  Decision  No.  76. 


1.  Auramin  (425,  426). 

21. 

Rhodamin   (496,  497,  498,  502,  504, 

2.  Naphthol  Yellow  S  (4). 

505). 

3.  Quinolin  Yellow  (666,  667). 

22. 

Acid  Magenta  (462). 

4.  Tartrazin  (94). 

23. 

Safranin  (583,  584,  585). 

5.  Acid  Yellow  (8,  88,  95,  4). 

24. 

The  Croceins  (13,  104,  106,  145,  151, 

6.  Spirit  Yellow  (Amidoazobenzol)  (7). 

160,  164,  169). 

7.  Curcumin  S  (399). 

25. 

Acid  Green  (434,  435). 

8.  Eosin  (512,  514,  515,  517,  521). 

26. 

Brilliant  Fulling  Green  (?). 

9.  Erythrosin  (516,  517). 

27. 

Malachite  Green  (427,  428). 

10.  Fluorescein  (510). 

28. 

Brilliant  Green  (428). 

11.  Orange  II  (86). 

29. 

Water  Blue  (480). 

12.  Crocein  Orange  (13). 

30. 

Patent  Blue  (440,  442). 

13.  Basic  Oranges  (?). 

31. 

Brilliant  Fulling  Blue  (?). 

14.  Fast  Red  (63,  65,  102,  103,  105, 

107, 

32. 

Domingo  Blue  B  extra  (?). 

144). 

33. 

Methyl  Violet  (451,  454). 

15.  Amara  Red  (?). 

34. 

Acid  Violet  (464,  465,  467,  468,  470, 

16.  Naphthol  Red  (?). 

471,  472,  474,  507). 

17.  Azo  red  (62). 

35. 

Bismarck  Brown  (197,  201). 

18.  Bordeaux  (65,  107,  157,  170,  171, 

198, 

36. 

Acid  Brown  (133,  138). 

244). 

37. 

Nigrosin  (600,602). 

19.  Victoria  Rubin  (?). 

38. 

Several  Acid  Blacks  (184  and  ?). 

20.  Ponceau  (13,  15,  44,  55,  56,  57, 

108, 

114,  146,  147,  148,  150,  160,  163 

L69, 

448). 

Of  these  38  titles  only  11  refer  to  a  single  entry  each  in  the  Green 
Tables  (namely  2,  4,  6,  7,  10,  11,  12,  17,  22,  28,  29);  7  titles  can  not 
be  definitely  connected  with  any  entry  in  the  Green  Tables  (titles  13 
15,  16,  19,  26,  31,  32);  one  title  is  broader  than  the  corresponding 
color  in  the  Green  Tables  (title  38)  and  the  remaining  19  titles  each 
and  all  refer  to  more  than  one  entry  in  the  Green  Tables. 


LISTS   OF    COLORS   RECOMMENDED   BY   INDIVIDUALS.  171 

These  31  titles  embrace  88  different  entries  in  the  Green  Tables; 
some  of  these  entries  are  included  in  two  or  more  titles  as  follows: 


Green  Table 

number.  Titles. 

4 2,5 

13 12,20,24 

65 14, 18 

107 14,18 


Green  Table 

number.  Titles. 

1G0 20,24 

169 20,24 

428 27,28 

517 8,9 


These  88  different  Green  Table  entries  can  be  divided  as  follows  on 
the  basis  of  the  compilation  of  literature  on  physiological  action  here- 
inbefore given  (see  p.  63) : 

Unfavorable  only.— 34,  164,  201,  425,  434,  502,  516,  602,  667.  Total  9,  or  10.2  per 
cent. 

Favorable  only.— 4,  65,  102,  103,  105,  107,  169,  399,  435,  462,  467,  512,  517,  521,  600. 
Total  15,  or  17.0  per  cent. 

Conflicting— -8,  13,  15,  55,  86,  88,  95,  106,  138,  160,  163,  197,  427,  428,  448,  451,  480, 
504,  584.    Total  19,  or  21.6  per  cent. 

Not  reported  on.— -7 ',  44,  56  \  57,  62,  63,  104,  108,  114,  133,  144,  145,  146,  147,  148, 
L50,  151,  157,  170,  171,  184,  198,  244,  426,  440,  442,  454,  464,  465,  468,  470,  471,  472,  174, 
496,  497,  498,  505,  507,  510,  514,  515,  583,  585,  666.     Total  45,  or  51  per  cent. 

According  to  this  mode  of  judging  only  15;  or  17  per  cent,  of  the 
colors  suggested  by  Ernst  for  food  coloring  would  be  regarded  as 
proper  for  use  in  foods. 

These  15  embrace  4  of  the  7  permitted  colors  of  Food  Inspection 
-ion  No.  76,  namely,  4,  107,  435,  and  517,  leaving  11  to  be  con- 
sidered.    Of  these,  5  were  not  on  the  United  States  market  in  the 
nier  of  1907,  namely,  102,  399,  467,  521,  and  600. 
The  remaining  6  are  as  follows  (the  numbers  in  parentheses  being 
the  number  of  sources  out  of  a  possible  12  offering  them  on  the  United 
States  market  in  the  summer  of  1907):  (jo  (2);  103  (6);  105  (1);  169 
(I);  462  (2);  and  512  (3). 

The  reasons  for  the  noninclusion  of  these  in  t ho  permitted  list  of 
1  Inspection  Decision  Xo.  76  have  been  given  on  page  167. 

MTJTTELET'S  INTERPRETATION  OF  THE  FRENCH  LAW. 

Muttelet  (Annales  des  Falsifications,  1909,  pp.  .   places  the 

;    Mowing  interpretation  on   the   French   regulations  <>f  December  29, 

0,  and  of  August   t.  L908,  classifying  them  as — 

I.  Those  colon  irhich  are  certainly  permitted  by  those  regulations. 
il.  Those  <«)l<.rs  whose  permitted  or  prohibited  use  i.->  doubtful. 
III.  Those  colon  which  arc  certainly  prohibited. 

The  Green  Table  numbers  contained  in  each  class  are  classified  as 

follows  (the  italicized  numbers  being  those  of  the  permitted  list  of 

i   Inspection   Decision   No.  76):   (a)   Unfavorably  reported;  (5) 

iSe*-  i  mis  r.r  Inotadlnc  Pi  I  List. 


172         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

favorably  reported;  (c)  conflictingly  reported;  (d)  not  reported  in 
the  literature  as  to  their  physiological  action  (see  p.  63) ;  in  paren-. 
theses  is  given  the  number  of  sources  out  of  a  possible  12  offering 
those  colors  on  the  United  States  market  in  the  summer  of  1907. 

I.  Those  colors  which  are  certainly  permitted: 

(a)  None.     (b)  4  (10);  5  (0);  462  (2);  512  (3);  517  (5);  520  (2);  600  (0);  total,  7. 
(c)  55  (2);  427  (2);  451  (5);  457  (0);  total,  4.     (d)  158  (0);  518  (2);  total,  2. 

II.  Those  colors  whose  permitted  or  prohibited  use  is  doubtful: 

(a)  None.     (6)  65  (2);  107  (7);  599  (0);  total,  3.     (c)  8  (5);  84  (2);  427  (2); 
457  (0);  601  (1);  total,  4.     (d)  452  (2);  456  (0);  513  (0);  514  (0);  total,  4. 

III.  Those  colors  which  are  certainly  prohibited: 

(a)  3  (0);  (b)  none;  (c)  427  (2);  (d)  none. 

It  will  be  noted  that  427  appears  in  all  three  of  Muttelet's  classifi- 
cations. The  reason  for  this  is  that  427  is  or  has  been  marketed  in  at 
least  three  different  forms;  of  these  the  straight  chlorhydrate  is  per- 
mitted, the  oxalate  and  the  zinc  chlorid  double  salt  are  of  doubtful 
admissibility,  and  the  picrate  is  undoubtedly  forbidden. 

Also  457  appears  in  Muttelet's  Classes  I  and  II  because  the  "Bleu 
Lumiere"  of  Muttelet's  Class  I  is  indistinguishable  from  his  "Bleu 
Lumiere"  of  Class  II,  when  using  the  Green  Tables  as  a  guide.  Fur- 
ther, this  list  of  Muttelet  contains  only  3  out  of  the  7  colors  permitted 
in  Food  Inspection  Decision  No.  76,  namely,  4  and  517  of  his  Class  I 
and  107  of  his  Class  II. 

An  inspection  of  Muttelet's  Class  I  discloses  13  Green  Table 
entries,  of  which  only  7  have  been  reported  in  the  literature,  as 
herein  compiled  and  rated,  in  a  favorable  manner;  of  these  7,  2  were 
not  on  the  United  States  market  in  the  summer  of  1907  and  of  the 
remaining  5,  2  are  in  the  permitted  list  of  Food  Inspection  Decision 
No.  76;  the  remaining  3  are:  462.  Acid  Magenta  (2);  512.  Eosin 
(3);  520.  Rose  Bengal  (2),  and  the  reasons  for  whose  noninclusion 
in  the  permitted  list  of  Food  Inspection  Decision  No.  76  have  been 
given  (p.  167). 

SECOND  INTERNATIONAL  WHITE  CROSS  CONGRESS. 

The  Second  International  White  Cross  Congress,  held  in  Paris, 
October  18  to  24,  1900,  according  to  the  Chemiker  Zeitung,  1909, 
page  1227,  adopted  the  following  list  of  colors  which  were  said  to  be 
proper  for  use  in  coloring  food  products.  Tho  figures  in  parentheses 
are  tho  Green  Table  numbers;  the  italicized  numbers  are  those  of  the 
permitted  list  of  Food  Inspection  Decision  \o.  76. 

5.  Fasl  Red  E  (106). 

6.  New  Coccin  (10(5). 

7.  Ponceau  2R  (66). 


1.  Erythronn  (616,  517). 

J.  lUiodaniin  B  (504). 

3.  Bordeaux  S  (107). 

4.  Bordeaux  G  (170). 


8.  Xylidin  Scarlet  (55). 


LISTS    OF    COLORS   RECOMMENDED   BY   INDIVIDUALS. 


173 


9.  Magenta  (448). 

10.  Acid  Magenta  (462). 

11.  Orange  I  (85). 

12.  Naphthol  Yellow  S  (4). 

13.  Chrysoin  (84). 

14.  Auramin  0  (425). 

15.  Acid  Green  (434,  435). 


16.  Lyons  Blue  (457). 

17.  Patent  Blue  (440,  442). 

18.  Paris  Violet  (451). 

19.  Acid  Violet  (464,  465,  467,  468,  470, 

471,  472,  474,  507). 

20.  Black  Indulins  (599). 

21.  Sulphonated  Nigrosin  (602). 


It  will  be  observed  that  titles  7  and  8  refer  to  the  same  Green  Table 
number;  this  leaves,  therefore,  only  20  titles  to  consider.  These  refer 
to  31  different  Green  Table  numbers  which  are  classified  as  (a)  only 
unfavorable  reports,  (b)  only  favorable  reports,  (c)  conflicting  reports, 
and  (d)  no  reports,  in  the  literature  hereinbefore  compiled  and  rated 
(see  p.  63) : 

(a)  425,  434,  516,  602;  total,  4. 

(b)  4,  85,  105,  107,  435,  462,  467,  517,  599;  total,  9. 

(c)  55,  84,  106,  448,  451,  457,  504;  total,  7. 

(d)  170.  440,  442,  464,  465,  468,  470,  471,  472,  474,  507;  total,  11. 

The  numbers  of  section  (b),  of  which  only  favorable  reports  are 
recorded,  are  the  only  ones  here  of  interest;  they  are  9  in  number,  or 
less  than  30  per  cent  of  all  those  included  in  tins  list,  and  of  these  9, 
5  are  on  the  permitted  list  of  Food  Inspection  Decision  No.  76.  The 
remaining  4  are  the  following,  the  number  in  parentheses  represent- 
ing the  number  of  sources  out  of  a  possible  12  offering  them  on  the 
United  States  market  in  the  summer  of  1907: 

105.  Fast  Red  E  (1). 

462.  Acid  Magenta  (2). 

467.  Acid. Violet  6  B,  not  offered. 

599.  Printing  Blue,  not  offered. 

The  reasons  for  the  noninclusion  of  these  colors  in  the  permitted 
list  of  Food  Inspection  Decision  No.  76  have  been  given  on  page  167. 

BEYTHXEN  AND  HEMPEL. 

Beythien  and  Hempel  (Farber  Ztg.,  1909,  v.  15,  pp.  301,  348,  392, 
436;  abst.  Ohem.  Ztg.,  1910,  p.  58)  recommend  the  following  colors 
for  use  in  food  products.  (The  numbers  in  parentheses  arc  the  corre- 
Bponding  Green  Table  numbers,  where  Buch  connection  could  be 
established;  the  italicized  numbers  are  those  of  the  permitted  list  of 
Food  Inspection  Decision  No.  76.) 


l.  AJiaarinblue  (682,  5G:J). 
l».  Amaranth  {107). 
:;.  Bordeaux  Red  (?). 
l.  Brilliant  Blw 
5.  Diamondfacfa 

i  Blue  ( •  898  MO). 

fellow  It  (9). 

I  Red  (68,  86,  102,   103,   LO 


512,  51  i.  515,  517,  521). 
116,  517). 
n.  FuchaiD  - 

12.  Light  Green  8  V  yellowiah  (435). 
IS.  Indigo  diaulphoacid    • 
li.  [nduli 

:  :ht  Blue 
it;.  Malachite  Green 
17.  Methyl  Violet  (451,  4 


174         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


18.  Xaphthol  Yellow  S  (4). 

26.  Roccellin  (102). 

19.  Orange  I  (85). 

27.  Roscellin  (?). 

20.  Orange  L  (54). 

28.  Rubin  (448). 

21.  Paris  Violet  (451). 

29.  Acid  Yellow  S  (4). 

22.  Phloxin  (518,  521). 

30.  Acid  Magenta  (462). 

23.  Ponceau  3R  (56,  57). 

31.  Solid  Blue  (?). 

24.  PoDceau  Red  (?). 

32.  Tropaeolin  OOO  (85,  86). 

25.  Primrose  (3,  513,  514). 

33.  Waterblue  (480). 

For  six  titles  (3,  4,  15,  24,  27,  and  31)  no  corresponding  Green 
Table  number  could  be  determined. 

Of  the  remaining  27  titles,  Xo.  9  includes  part  of  No.  10,  32  includes 
19,  9  includes  part  of  25,  8  includes  26,  17  includes  21,  11  is  identical 
with  30,  and  18  is  identical  with  29,  all  on  the  assumption  that  the 
correct  connections  between  title  and  Green  Table  numbers  have  been 
made.  Therefore  these  27  titles  are,  in  fact,  only  25  titles;  of  these 
25  titles,  13  refer  to  but  one  Green  Table  number  each;  the  remaining 
12  titles  each  refer  to  two  or  more  Green  Table  numbers. 

The  Green  Table  numbers  above  given  are  now  arranged  in  the 
following  four  classes  according  to  the  literature  hereinbefore  com- 
piled and  rated  (see  p.  63) : 

(a)  Only  unfavorable  reports:  3,  516,  639;  total,  3. 

(b)  Only  favorable  reports:  4,  65,  85,  102,  103,  105,  107,  435,  462,  477,  512,  517,  521, 
599,  692;  total,  15. 

(c)  Conflicting  reports:  9,  86,  427,  428,  448,  451,  480,  563,  601;  total,  9. 

(d)  No  reports:  54,  56,1  57,  63, 144,  454,  513,  514,  515,  518,  562,  603,  640;  total,  13. 

The  15  Green  Table  numbers  of  class  (b)  are  the  only  ones  here  of 
interest;  they  include  6  out  of  the  7  permitted  colors  of  Food  Inspec- 
tion Decision  76;  of  the  remaining  9,  4  (102,  477,  521,  599)  were  not 
on  the  United  States  market  in  the  summer  of  1907.  The  remaining 
5  are  as  follows.  (The  number  in  parentheses  is  the  number  of 
sources  out  of  a  possible  12  offering  them  on  the  United  States 
market  in  the  summer  of  1907): 

65.  Fast  Red  B  (2).  462.  Acid  Magenta  (2). 

103.  Azorubin  S  (6).  512.  Eosin  (3). 

L05.   Fast  Red  E  (1). 

The  reasons  for  the  noninclusion  of  these  colors  in  the  permitted 
list  of  Food  Inspection  Decision  Xo.  76  have  been  given  on  page  167. 

SUMMARY  OF  THREE  PRECEDING  RECOMMENDATIONS. 

The  recommendations  made  by  Ernst,  the  White  Gross  Congress, 
and  Beythien  and  Hempel  are  summarized  in  the  following  table: 


i  if  permitting  qm  of  Ponceau  SB, 


LISTS    OF    COLOKS    RECOMMENDED    BY   INDIVIDUALS. 


175 


Summary  of  recommendations  from  three  sources. 


Green 

Table  No. 

(11). 

Unfavorable  reports  only. 

Number 
recom- 
mending. 

Dealers 
offering. 

Ernst. 

White 
Cross. 

Beythien 

and 
Hempel. 

3 

x                     1 

0 
6 
0 
2 
3 
1 
-' 
1 
i) 
0 
1 

94 

104 

201 

425 

434 

502 

510 

002 

039 

X 
X 
X 
X 
X 
X 
X 
X 

1 
1 
1 
2 
2 
1 
3 
2 
1 

X 
X 

X 

X 

X 

X 

007 

Total .  . 

X 

9 

4 

3 

Green 

Table  No. 

(19). 

Favorable  reports  only. 

Number 
recom- 
mending. 

Dealers 
offering. 

Ernst. 

White 
Cross. 

Beythien 

and 
Hempel. 

4 

05 

85 

X 

X 

X 

X 
X 
X 
X 
X 
X 
X 

3 

2 
2 
2 
2 
3 
3 

3 
3 

2 
1 

2 
3 
2 
2 

1 
1 

10 
2 
2 
0 
0 
1 
7 
1 
0 
4 
2 
0 
0 
3 
5 
0 
0 
0 
3 

X 

102 

103 

105 

107 

109 

399 

435 

482 

467 

477 

X 
X 
X 
X 
X 
X 
X 
X 
X 

X 
X 

X 
X 
X 

X 
X 

X 
X 
X 
X 
X 

512 

517 

521 

599 

X 
X 
X 

X 

X 

000 

692 

X 

X 

Total.. 

15 

9 

15 

Green 

Tab!.-  No. 
(21). 

Conflicting  reports. 

Numl>er 
recom- 
mending. 

I><':i!it-; 
oilering. 

Ernst. 

White 

Cross. 

Beythien 

ami 
Hempel. 

8 x 

l 

l 
1 

1 

l 

■_> 

l 
l 

l 

l 
l 
l 
•j 

3 
I 

1 

5 

1 
0 
0 

2 

H 
0 

I 

0 
0 
0 
4 
2 
3 
4 
5 
0 
1 
5 
0 
1 

X 

13 

16 

5.-. 

VI 

X 
X 
X 

X 

1 

86 





106 

138 

100 

183 

197 

4J7 

• 

461. 

X 
X 
X 
X 
X 
X 
X 

X 

X 

\ 

X 

X 

X 

\ 

X 

X 
X 

668. 

X 

X 

684. 

0<)1 

X 

I'l 

7 

9 

176 


COAL-TAR   COLORS   USED  IN   FOOD   PRODUCTS. 
Summary  of  recommendations  from  three  sources — Continued. 


Green 
Table  No. 

(51). 

Not  reported 

on. 

Number 
recom- 
mending. 

Dealers 
offering. 

Ernst. 

White 
Cross. 

Beythien 

and 
Ilempel. 

7 

44 

54 

X 
X 

2 
2 

2 
2 
2 
2 
2 
2 
2 
1 
1 
1 
1 
2 

1 

2 
2 

1 
1 
1 

1 

1 

0 

0 
1 
1 
0 
0 
0 

1 

2 
0 
0 
0 
0 
2 
0 
0 
0 
0 
0 
0 
0 
0 
0 
0 
0 

1 

0 
0 

1 

0 

0 
0 
0 
0 
0 
0 
0 
0 
0 
4 
0 
0 
0 
2 
0 
0 
0 
0 
0 
0 

X 

X 
X 

56 

57 

62 

63 

104 

108 

114 

133 

144 

145 

146 

147 

148 

150 

151 

157 

170 

171 

184 

198 

244 

426 

440 

442 

454 

464 

465 

468 

470 

471 

472 

474 

496 

497 

498 

505 

*07 

510 

513 

X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 
X 

X 

X 

X 

X 
X 

X 

X 

X 
X 
X 

X 
X 
X 

X 

X 

X 
X 
X 
X 

514 

515 

518..    . 

X 
X 

562 

583 

586 

603 

X 
X 

X 

X 

840..   . 

866 

Total.. 

X 

1 

45 

11 

13 

r 

These  three  recommendations  embrace  105  different  Green  Table 
numbers.  The  following  table  discloses  the  conformity  of  the  com- 
posite of  these  three  recommendations  to  the  United  States  market 

in  lite  summer  of  1907: 

Number  of  suggested  samples  in  the  three  supplementary  lists  found  on  the  market,  1907. 


Data 

1  in 

on  1   | 
States 

market. 

l'n  favorable 

11 
l'.t 
M 

.M 

7 
13 

17 

in 

Total 

105 

47 

LISTS   OF   COLORS   RECOMMENDED  BY  INDIVIDUALS.  177 

UNPUBLISHED   RECOMMENDATIONS   OF   A  MANUFACTURER. 

In  addition  to  these  published  recommended  lists  the  following 
recommendation  has  been  made  by  letter  by  a  manufacturer  who 
contributed  specimens  of  food  colors  to  the  United  States  market 
in  the  summer  of  1907: 

That  for  the  following  permitted  colors  of  Food  Inspection  Decision 
No.  76,  there  be  substituted  certain  colors,  the  Green  Table  numbers 
alone  being  here  given : 


rmitted. 

Substitute 

4 

94 

56 

53 

85 

15 

517 

521 

In  regard  to  these  proposed  substitutes  it  is  to  be  said  that  Xos. 
15  and  521  were  not  on  the  United  States  market  in  the  summer  of 
1907,  according  to  the  canvass  made  and  described  in  Section  I, 
Nos.  53  and  94  were  on  that  market,  No.  53  had  not  been  examined 
physiologically,  and  No.  94  had  been  examined  physiologically 
with  only  unfavorable  results.  The  way  was,  therefore,  not  open  to 
placing  any  of  these  colors  on  the  permitted  list  under  the  procedure 
adopted.  However,  had  No.  15  been  on  the  market  it  would  not 
have  been  placed  on  the  permitted  list,  because  it  has  been  examined 
physiologically  with  contradictory  results,  while  No.  521  might  have 
been  placed  on  the  permitted  list  because  it  seems  to  have  been 
examined  physiologically  and  with  only  favorable  results. 

BEHAL. 

As  the  result  of  careful  investigation  Belial  {Revue  Generale  des 
Matieres  Colorantes,  1010,  p.  131)  suggests  the  use  of  21  definite 
chemical  individuals  which  are  given  in  the  following.  With  the 
tabulation  on  page  63  as  a  guide  these  21  colors  are  classified  as 
unfavorable,  favorable,  contradictory,  and  not  reported  on.  The 
italicized  figures  are  in  the  permitted  list  of  Food  Inspection  Decision 
No.  76. 

UNFAVORABLE  (1). 

425.  Auramin  0  (S). 

FAVORABLE  (11). 


Naphthol  Xell<m  8  (10). 
lordeaui  B 
Orange!  (2). 

Red  (1). 

Amarainh 

Light  Green  s  r  y.  Hon  i  b    \ 
97291°— Bull.  117—12 12 


Acid  Magenta  (2). 
407,  A<-i<l  Violet  SB  (none). 
512.  i:    In 

Eiythroein 

520.  i;  .1  (2). 


178 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 


CONTRADICTORY  (6). 


55.  Ponceau  2  R  (2). 
84.  Chrysoin  (2). 
106.  NewCoccin  (5). 


54.  Scarlet  R  (1). 

64.  Crystal  Ponceau  (1). 


427.  Malachite  Green  (2). 
451.  Methyl  Violet  (5). 
480.  Water  Blue  (1). 


NOT  REPORTED    ON    (3). 


440.  Patent  Blue  (1). 


The  five  in  the  " favorable"  list  which  were  on  the  United  States 
market  in  the  summer  of  1907,  but  are  not  in  the  permitted  list  of 
Food  Inspection  Decision  No.  76,  namely: 


65.  Bordeaux  B  (2); 
105.  Fast  Red  (1); 
462.  Acid  Magenta  (2); 


512.  Eosin  (2); 

520.  Rose  Bengal  (2), 


are  tinctorially  provided  for  in  that  list;  only  one  of  the  21  colors 
recommended  by  Belial  was  not  on  the  market  of  the  United  States 
in  the  summer  of  1907,  namely,  467  Acid  Violet  6B,  and  this  is  in  the 
"favorable"  list.  The  reasons  for  the  non-inclusion  of  these  colors 
are  given  on  page  167. 

CONCLUSIONS. 

It  is  clear  from  an  inspection  of  the  preceding  analysis  of  the  six 
lists  just  given  that  the  confusion  referred  to  on  page  165  as  existing 
in  the  three  recommendations  made  before  the  formulation  of  the 
permitted  list  of  Food  Inspection  Decision  76  is  not  at  all  diminished 
by  these  six  lists  published  after  the  announcement  of  that  decision, 
as  is  shown  in  the  following  table : 

Analysis  of  six  lists  published  after  the  issuance  of  F.  I.  D.  76. 


Total  of 

dyes 
wanted. 

Reports  on  physiological 
effect  . 

l'hysio- 
logica] 
effect 
not  re- 
ported. 

Number 

of  dyes 
wanted 

List  of— 

Unfavor- 
able. 

Favor- 
able. 

Contra- 
dictory. 

and  con- 
tained in 
F.  I.  I). 
76. 



88 

7 
81 
40 

4 
21 

9 

15 

7 

15 

1 
[1 

19 

45 

•i 

White  (  ro            

I 
3 

1 

7 
9 
1 
0 

11 

u 

1 
3 

1 5c,  t  liicn  and   11  fin  pel 

afahufad  urer 

Iir-ii;ii 

The  Bame  wide  differences  of  opinion  as  fco  the  Four  points  discussed 
on  page  166  not  only  continue  but  arc  accentuated. 


179 

XIV.  CHEMICAL  EXAMINATION  OF  THE  SEVEN  PERMITTED 

COLORS,  1907. 

NEED  OF  CHEMICAL  CONTROL. 

The  most  striking  thing,  from  the  chemist's  point  of  view,  in  the 
literature  relative  to  the  physiological  action  of  coal-tar  colors,  is 
the  almost  universal  absence  of  the  results  of  chemical  examination  or 
identification  of  the  materials  subjected  to  physiological  test.  There 
is  hardly  any  description  or  statement  of  the  strength  or  the  con- 
centration of  the  materials  examined,  or  of  the  amount  or  nature  of 
materials  not  coloring  matter  present  in  the  substances  subjected 
to  these  physiological  tests.  It  is  true  that  some  publications  give 
identification  tests,  but  few  assert  the  identity  of  the  material 
subjected  to  certain  physiological  tests,  with  the  description  so  given. 

The  need  for  some  such  chemical  control  as  to  identity  and  quality 
must  be  apparent  to  all  having  experience  with  the  commercial 
varieties  or  grades  of  coal-tar  colors.  Many  of  these  commercial 
brands  of  coal-tar  colors  contain  added  coloring  matter  other  than 
the  principal  constituent  for  the  purpose  of  correcting  some  defect 
unavoidably  arising  during  the  manufacture.  Where  those  com- 
mercial brands  are  sold  for  textile  and  other  manufacturing  purposes 
there  is  no  valid  objection  to  such  practice,  because  in  such  uses  the 
tinctorial  properties  and  effects  of  the  commercial  brands  are  the  tilings 
the  buyers  desire  and  pay  for,  and  the  exact  nature  of  the  materials 
accomplishing  the  results  is  in  reality  of  secondary  importance; 
but  when  coal-tar  colors  are  to  be  used  in  foods,  and  in  addition  to 
tinctorial  effect  the  absence  of  any  physiological  action  is  necessary, 
it  La  at  least  of  doubtful  propriety  to  market  such  corrected  or  adjusted 
brands  unless  the  correction  or  the  adjustment  be  made  with  harmless 
colors. 

There  are  a  few  instances  in  the  relevant  literature  where  it 
attempted  to  explain  the  different  results  attained  by  observers  by 
the  difference  in  the  composition  of  the  materials  subjected  to  pi. 
Logical  test,  and  there  are  other  instances  showing  the  difficulties 
encountered  in  obtaining  specimens  of  coal-tar  colors  which  would 
always  give  favorable  physiological  result. 

The  variation  in  composition  of  coal-tar  colors  may  be  exemplified 
by  the  following  excerpts  from  the  literature: 

l.  Weyl  (y.  91)§  di  the  dim  between  his  results  and 

those  of  Oazeneuve  and  L6pine  with  Naphthol  Yellow  s,  stat< 

folio 

Ii  is  to  be  noticed,  how*  •  that  the  Naphthol 

YeUo  nine  NS  that  they  probably  experim 


180         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

with  another  substance.  My  own  investigations  were  made  on  dogs  with  a  preparation 
for  which  I  am  indebted  to  the  kindness  of  Dr.  G.  Schultz,  of  the  Aniline  Manufactur- 
ing Co.  of  Berlin.     It  was  purified  by  precipitation  and  recrystallization. 

2.  Fraenkel  (p.  578)  expresses  the  opinion  that  the  harmful  results 
observed  with  Metanil  Yellow  (95  of  the  Green  Tables)  may  be  due  to 
diphenylamin  contained  in  the  color,  which  diphenylamin  may  be 
a  decomposition  product  of  the  Metanil  Yellow,  particularly  since,  as 
Weyl  states  (p.  130),  it  "smelled  strongly  of  diphenylamin." 

3.  PfefTer  ( UnterscJiungen  aus  dem  Botanischen  Institut  zu  Tuebin- 
gen,  Vol.  II,  p.  186)  says: 

In  repeating  my  experiments  I  beg  that  it  be  considered  that  differences  in  observa- 
tion may  be  caused  by  the  quality  of  the  coloring  matters.  For  quite  apart  from  the 
fact  that  the  coloring  matters  are  in  part  variable  mixtures  of  various  compounds,  and 
not  infrequently  contain  foreign  admixtures,  the  quality  of  the  goods  brought  into 
market  may  change  from  time  to  time.  Thus  formerly  magenta  was  the  acetate, 
whereas  to-day  it  is  the  hydrochlorid.  Also  foreign  admixtures  may  be  poisonous  or 
may  exert  no  influence  on  the  absorption  of  color. 

4.  Stilling  (ArcUv.  Exper.  Path.  Pharm.,vol  28,  1891,  p.  852)  says: 

With  respect  to  the  blue  pyoctanin,  I  have  during  the  entire  time  been  engaged 
in  ascertaining  the  most  effective.  The  things  marketed  by  E.  Merck  as  P.  cceruleum 
have  therefore  now  become  uniform  and  homogeneous,  which  could  not  be  the  case 
at  the  beginning.  The  P.  coeruleum  now  furnished  by  E.  Merck  is  the  hydrochlorid 
of  pure  hexamethylpararosanilin. 

The  variable  degrees  of  purity  attained  by  products  of  this  kind 
on  the  market  was  apparently  the  first  cause  of  the  prohibition  by 
the  German  Government  of  the  coal-tar  color  known  as  Corallin  for 
use  in  food  products — not  because  Corallin  itself  was  harmful,  but 
because  in  the  manufacture  of  this  product  it  was  so  apt  to  retain  im- 
purities which  in  and  of  themselves  produced  bad  effects,  so  that  this 
particular  color  was  specifically  excluded  by  the  German  Government. 

In  a  few  cases  it  is  stated  that  the  substance  subjected  to  physio- 
logical test  had  been  purified,  but  these  descriptions  are  hardly  such 
as  to  enable  others  to  arrive  at  substantially  the  same  result  with 
reasonable  certainty. 

5.  Stilling  in  his  monograph  entitled  Anilin  FarbstofTe  als  Anti- 
septica  (Strassburg,  1890,  Pt.  I,  p.  16)  says: 

The  foregoing  (relative  to  the  action  of  Methyl  Violet  on  the  eyes  of  rabbits)  holds 
only  for  pure  substances.  Many  anilin  colors  of  otherwise  very  antiseptic  properties 
are  contaminated  with  arsenic,  particularly  (he  otherwise  useful  Ethyl  Violet.  With 
such  substance  serious  poisonings  and  death  can  be  produced  in  experimental  animals. 

6.  Stilling  in  Part  II  of  the  same  monograph,  pages  5  and  6,  says: 
Such  substances  I  coal-tar  colon)  must  lie  chemically  pure  and  can  not,  for  example, 

bo  any  mixture  of  various  blue  or  violet  dyes.      There  is  therefore  a  great  difference 

whether  a  substance  be  tested  only  bacteriologically  or  also  in  addition  physiologically 
and  therapeutically.    Two  preparations  may  be  antiseptically  wholly  equal,  but  the 

one  preparation  may  contain  harmful  admixtures  which  produce  violent  irritations. 


ANALYSIS   OF   PERMITTED   COLORS,   1907.  181 

7.  Thus  Weyl,  speaking  of  his  Metanitrazotin  (p.  120),  describes 
the  purification  method  as  follows : 

It  is  dissolved  in  warm  alcoholic  solution  of  sodium  hydroxid  filtered  and  precipi- 
tated with  hydrochloric  acid.  The  precipitate  is  freed  from  the  adhering  liquid  by 
the  aspirator  and  washed  with  hot  water. 

8.  Weyl  says  of  his  Metanil  Yellow  (p.  130): 

For  purification  the  color  was  dissolved  in  water  filtered  and  separated  by  the 
addition  of  sodium  acetate.  The  yellow  mass  was  freed  from  the  adherent  liquid  by 
the  filter  pump  and  dissolved  in  hot  alcohol,  in  which  it  is  difficultly  soluble,  and 
obtained  from  this  in  the  form  of  yellow  crystals.  The  material  used  for  the  experi- 
ment was  almost  pure,  as  the  following  analytical  statement  shows:  0.4895  gram  of 
the  color  dried  in  105°  gave  0.084  sodium  sulphate.  Sodium  required,  6.1;  found,  5.6. 
(Note. — This  amounts  to  91.8  per  cent  of  theory.) 

9.  Weyl  (Zts.  Hygiene,  1889,  Vol.  II,  p.  34,  On  Safranin 
Poisoning)  describes  the  difficulties  he  had  in  obtaining  safranin  on 
the  market  that  was  clean  or  pure;  all  preparations  were  free  from 
arsenic,  and  contained  small  amounts  of  iron,  chlorin,  and  traces 
of  chromium.  In  one  specimen  the  ash  amounted  to  4.8  per  cent. 
The  theoretical  percentage  of  nitrogen  in  pure  safranin  is,  according 
to  Weyl,  15.3  per  cent;  in  two  commercial  products  he  found  12.7 
and  12.3  per  cent,  respectively  (83  and  80.4  per  cent  of  theory); 
he  recrystallized  the  specimen  containing  12.7  per  cent  twice  from 
dilute  hydrochloric  acid;  the  first  recrystallization  produced  a  speci- 
men containing  13.8  per  cent  (90.2  per  cent  of  theory)  of  nitrogen; 
the  second  recrystallization  produced  a  substance  containing  14 
per  cent  (91.5  per  cent  of  theory)  nitrogen. 

10.  Chlopin  in  his  book  (p.  110)  says: 

Nevertheless,  each  dye  was  tested  by  me  personally  with  the  usual  reagents  and 
the  dyeing  of  fabric  in  order  to  avoid  the  confounding  of  one  dye  with  another.  I 
convinced  myself,  from  my  experience,  that  not  only  druggists  but  the  home  offices 
of  the  makers  occasionally  send  dyes  which  do  not  correspond  to  the  requirements 
and  resemble  them  only  in  name. 

(Page  114.)  All  the  dyes,  which  according  to  my  experiments  proved  to  be  pois- 
.  were  carefully  examined  iW  contents  of  arsenic,  chromium,  and  injurious 
metals,  and  were  found  to  be  free  from  these  admixn 

FIRST  METHODS  OF  ANALYSIS  USED. 

In  the  summer  of  1907  there  were  OD  the  United  State-  market  30 
different  specimens  of  the  seven  permitted  colors  of  Food  Inspection 
Decision  No.  7G.  A  chemical  examination  of  those  •"><)  specimens 
would  disclose  the  qualitative  conditions  of  the  market  so  far  as 
these  seven  permitted  colors  were  concerned,  and  it  was  expected 
thai  certain  limits  for  standards  of  cleanliness  would  he  fixed  by 

such  an  examination. 


182         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

In  examining  these  30  specimens  of  the  seven  permitted  colors 
chemically  the  following  determinations  were  made: 

1.  Moisture. 

2.  Chlorin  as  chloride. 

3.  Sulphated  ash,  together  with  its  iron,  aluminum,  calcium,  and  copper  content, 
and  the  determination  of  the  sulphuric  acid  in  the  sulphated  ash. 

4.  Total  sulphur. 

5.  Gutzeit  test  (test  17  of  the  United  States  Pharmacopoeia,  eighth  revision). 

6.  Heavy  metals  test  (test  121  of  the  United  States  Pharmacopoeia). 

7.  Total  insolubles,  together  -with  the  determination  of  the  proportion  that  is  vola- 
tile on  ignition. 

8.  Ether  extractive. 

The  methods  of  analysis  actually  used  on  these  30  dye  specimens 
are  here  given  solely  for  the  purpose  of  comparing  them  with  the 
methods  developed  therefrom  and  presented  beginning  with  page  210. 
Experience  has  shown  that  the  methods  here  given  are  defective  in 
many  particulars,  and  therefore  they  are  not  to  be  used  for  exact 
work. 

MOISTURE. 

Dry  a  sample  of  each  color  weighing  3  grams  at  105°  to  108°  C.  for  two  hours.  The 
loss  in  weight  is  assumed  to  be  moisture. 

This  method  is  not  wholly  accurate  in  the  case  of  Naphthol  Yellow,  nor  is  it  accu- 
rate in  the  case  of  Amaranth;  but  the  scarcity  of  material  made  it  seem  unwise,  at 
this  stage,  to  undertake  any  extended  investigation  as  to  the  amount  or  nature  of  the 
heating  required  surely  to  expel  all  moisture.  The  results,  therefore,  while  not  as 
accurate  as  might  be  desired,  are,  for  the  purposes  of  this  exploratory  investigation, 
sufficiently  accurate  for  the  object  for  which  they  were  undertaken. 

CHLORIN    AS    CHLORIDS. 

Gently  heat  samples  weighing  0.1  gram  with  2  grams  of  sodium  carbonate,  and  after 
destroying  the  greater  part  of  the  organic  matter  add  0.1  gram  of  powdered  potassium 
nitrate  and  gently  heat  the  whole  until  the  organic  matter  is  entirely  destroyed. 
After  cooling  treat  the  whole  with  small  amounts  of  cold  water  and  remove  from  the 
crucible;  effect  the  solution  of  the  whole  by  gently  heating.  After  cooling  bring  the 
bulk  to  about  150  cc,  cool  to  room  temperature,  slightly  acidify  with  nitric  acid,  pre- 
cipitate the  chlorin  with  silver  nitrate,  and  weigh  as  silver  chlorid. 

SULPHATED    ASH. 

Moisten  half-gram  samples  with  concentrated  sulphuric  acid,  gently  evaporate  to 
dryness,  and  treat,  the  residue  with  5  cc  of  concentrated  sulphuric  acid  and  again 
evaporate  to  dryness;  repeat  the  operation  until  a  white  ash  results,  when  the  whole 
is  ignited  1<>  constant  weight.  After  weighing  take  up  the  sulphated  ash  in  boiling 
water  (and  if  necessary,  any  undissolved  material  can  be  taken  up  with  hydrochloric 
acid  by  treatment  on  a  boiling-water  bath.)  Mix  the  two  solutions  and  bring  to  a 
total  volume  of  200  cc.  In  one  half  thereof  determine  the  contained  sulphur  by  a 
precipitation  with  barium  chlorid,  and   weigh  BS  barium  sulphate;   in  the  other  half 

determine  iron  and  aluminum  by  precipitation  with  ammonia,  ignite  and  weigh  ;is 

ferric  and  aluminum  oxid.     No  separation  of  any  contained  aluminum  was  under- 


ANALYSIS   OF   PERMITTED   COLORS,   1907.  183 

taken  in  the  nitrate  from  the  iron;  the  lime  was  precipitated  as  oxalate.  In  the  only 
rase  that  copper  was  encountered  it  was  precipitated  as  sulphid  before  taking  out  the 
iron  or  the  calcium. 

TOTAL   SULPHUR. 

Mix  0.2  gram  of  the  sample  with  4  grams  of  sodium  carbonate  and  0.5  gram  of  potassium 
nitrate,  and  ignite  to  complete  the  destruction  of  the  organic  matter;  take  up  in  hot 
water;  acidify  with  hydrochloric  acid  and  precipitate  the  sulphur  as  barium  sulphate 
with  barium  chlorid. 

GUTZEIT   TEST. 

Mix  2  grams  of  the  substance  with  2  grams  of  a  mixture  of  1  part  of  potassium  nitrate 
and  5  parts  of  sodium  carbonate  and  ash  in  a  porcelain  crucible  over  a  low  flame;  if 
not  white  when  cool,  mix  the  ash  with  1  gram  of  potassium  nitrate  and  again  ash  over 
a  low  flame.  Generally  the  second  ashing  is  sufficient.  Dissolve  the  residue  in  50 
cc  of  hot  water,  boil,  filter,  neutralize  with  dilute  sulphuric  acid,  and  evaporate  to 
substantial  dryness  on  a  boiling-water  bath.  Then  add  1  cc  of  concentrated  sulphuric 
acid  and  dry  over  a  Bunsen  flame;  take  up  the  residue  with  5  cc  of  distilled  water 
containing  0.5  cc  of  concentrated  sulphuric  acid  and  10  cc  of  a  saturated  solution  of 
sulphurous  acid;  evaporate  the  whole  to  a  bulk  of  5  cc  on  a  water  bath;  add  20  cc  of 
8  per  cent  hydrochloric  acid  and  subject  this  material  to  the  action  of  2  grams  of  metallic 
zinc,  free  from  arsenic,  which  has  been  so  activized  by  means  of  platinic  chlorid  that 
at  the  end  of  two  hours  more  than  1  gram  of  zinc  has  dissolved  and  the  evolution  of 
gas  has  been  constant  and  continuous.  Conduct  the  reaction  in  a  flask  of  60  cc  capacity 
with  a  neck  1  cm  in  diameter  and  6  cm  long.  After  the  introduction  of  the  solution  and 
the  zinc  into  the  flask,  stopper  the  neck  of  the  bottle  with  gauze,  the  lower  half  of 
which  is  dry  and  the  upper  half  moistened  with  the  test  solution  of  lead  acetate  of 
the  United  States  Pharmacopoeia.  After  carefully  wiping  the  lip  of  the  fla'sk,  cover 
it  with  Schleicher  &  Schiill  quantitative  filter  paper  which  has  been  saturated  three 
times  with  alcoholic  mercuric  chlorid  solution,  with  complete  drying  between  each 
saturation  on  one  and  the  same  spot  of  the  filter  paper. 

In  the  case  of  Naphthol  Yellow  S  it  is  necessary  to  heat  gently  with  10  grams  of 
sodium  carbonate  until  the  organic  matter  is  substantially  all  destroyed,  then  add 
1.5  grams  of  potassium  nitrate  and  heat  to  complete  destruction  of  the  organic  matter. 
Dissolve  the  fused  mass  in  hot  water  and  a  few  drops  of  fifth-normal  sulphuric  acid; 
then  make  distinctly  acid  with  the  same  and  add  an  excess  of  1  cc  of  concentrated 
sulphuric  acid;  evaporate  first  on  the  water  bath  and  afterwards  on  asbestos  until  all 
odor  of  nitrous  fumes  and  of  hydrochloric  acid  has  disappeared.  Take  up  the  residue 
in  5  CC  of  water  and  15  cc  of  a  saturated  solution  of  sulphurous  acid  in  water.  Beat 
the  whole  on  the  water  bath  until  no  odor  of  sulphur  dioxid  remains. 

The  preparation  of  the  sample  by  ignition  with  carbonate  and  nitrate  should  not 
bedone  in  platinum,  butshould  be  done  in  a  porcelain  crucible,  since  it  has  hap; 
thai  as  much  as  0.05  mg  of  arsenic  mixed  with  the  dye,  which  had  been  fused  in 
platinum  with  carbonate  and  nitrate,  could  not  be  detected  on  the  mercury-chlorid 

paper,  whereas  0.01  mg  when  similarly  treated  in  porcelain  could  always  DO  detected, 
and  0.006  mg  would  usually  be  found  when  done  in  porcelain. 

HEAY1     ICBTALS. 

Mix  as  much  Oi  the  BUDfltance  as  approximately  contains  1  gram  «'f  color  with   10 

times  its  we  i -ht  of  carbonate  of  soda  and  Ignite  with  the  addition  tnoi  potas- 

sium nitrate.     Dissolve  the  whole  in  water,  any  u:  1  being  taken  up 


184         COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

with  hydrochloric  acid,  bring  the  two  solutions  together  and  slightly  acidify  with 
hydrochloric  acid;  dilute  to  100  cc;  place  10  cc  in  a  test  tube  of  40  cc  capacity  and 
warm  to  50°  C.  in  a  water  bath;  add  10  cc  of  a  freshly  prepared  saturated  solution  of 
hydrogen  sulphid  in  water,  stopper  the  test  tube  well  and  allow  the  whole  to  stand 
in  water  having  a  temperature  of  35°  C.  for  a  half  hour.  Dilute  a  3.3  cc  portion  to  10  cc, 
treat  as  before  with  10  cc  of  hydrogen  sulphid  in  water  for  one-half  hour  at  35°  C,  and 
add  to  each  ammonium  hydrate. 

TOTAL   INSOLUBLES. 

Dissolve  1  gram  of  the  substance  in  1  liter  of  water,  filter  through  counterpoised 
quantitative  filters,  and  wash  with  hot  water  until  all  traces  of  color  are  removed 
from  the  filter  paper,  then  dry  at  100°  C.  to  constant  weight  and  weigh;  report  the 
weight  as  total  insolubles.  Ignite  the  total  insolubles  in  a  platinum  crucible  and  report 
the  residue  remaining  as  nonvolatile  insolubles. 

ETHER   EXTRACTTVE. 

Two  methods  were  employed,  the  one  consisting  in  direct  extraction  of  the  sub- 
stance in  a  Soxhlet  apparatus  by  means  of  redistilled  ether  dried  over  sodium. 
Schleicher  &  Schull  extraction  cartridges  were  used  after  they  had  been  thoroughly 
extracted  by  ether  and  shown  by  examination  that  they  yielded  no  extractive  to 
ether  whatever.  This  is  a  necessary  precaution,  because  the  amount  of  ether  extrac- 
tive matter  in  these  cartridges  varies.  The  amount  of  ether  extractive  was  determined 
by  driving  off  the  ether  over  a  32-candlepower  incandescent  lamp,  finally  drying  and 
cooling  in  a  desiccator. 

This  method,  however,  is  not  satisfactory,  since  the  results  it  gives  are  undoubtedly 
low  and  it  seems  that  the  higher  the  material  was  dried  the  more  erratic  were  the 
results.     Therefore  the  following  method  was  used: 

Disolve  1  gram  of  the  sample  in  100  cc  of  water;  add  0.5  gram  of  sodium  acetate; 
extract  three  times  with  50  cc  of  ether  in  aseparatory  funnel;  mix  the  ether  so  recov- 
ered with  10  cc  of  water;  separate  the  ether  and  dry  with  fused  calcium  chlorid;  let 
stand  from  12  to  24  hours;  pour  off  from  the  calcium  chlorid;  distil  off  the  ether  as 
in  the  preceding  method;  acidify  the  color  solution  containing  sodium  acetate  with 
1  cc  concentrated  hydrochloric  acid;  extract  three  times  with  50  cc  of  ether,  and 
proceed  as  before. 

RESULTS  OF  CHEMICAL  EXAMINATION,  1907. 

DETAILED    CHEMICAL   DATA    OX    EACH    PERMITTED   COLOR. 

The  results  of  this  examination  are  given  in  the  following  tabula- 
tions under  the  respective  Green  Table  numbers;  the  serial  num- 
bers refer  to  the  numbers  assigned  to  the  specimens  as  they  were 
received.  The  abbreviations  "p."  and  "n.  p."  opposite  "Gutzeit 
test,"  and  "Heavy  metals  test"  stand  for  "pass,"  and  "not  pass," 
respectively,  according  as  the  specimen  did  or  did  not  comply  with 
those  requirements;  the  entries  opposite  "Ratio,"  indicate  the  degree 
of  concordance  of  the  sulphated  ash  as  weighed,  and  tho  contained 
SO,  calculated  back  to  sodium  sulphate  and  is  a  measure  of  tho  accu- 
racy or  dependability  of  the  sulphated  ash  item  audits  determination. 


ANALYSIS   OF   PERMITTED   COLORS,    1907. 


185 


As  a  guide  in  ascertaining  the  conformity  of  these  colors  to  their  sup- 
posed standards  when  judged  by  the  analytical  data  obtained,  the 
following  table  may  of  service: 


Percentages  of  sulphur,  sodium,  and  sulphated  ash  properly  belonging  to  each  of  the  seven 

permitted  colors. 


Green 

Table 
No. 


4 
56 
85 
107 
435 
517 
692 


Name  of  colors. 


Sulphur. 


Naphthol  Yellow 

Ponceau  3  R 

Orange  I 

Amaranth...  

Light  Green 

Erythrosin 

Indigotin 


8.95 
12. 97 

9.16 
15. 92 

11.12 
(') 
13.75 


Sodium. 


1  Iodin  in  No.  5Vt 


.7  per  c?nt. 


12.87 
9.  33 
6.58 

11.44 
8.31 
5.24 


Sul- 
phated 
ash. 


39.73 

20.31 
35.32 
25.64 
16.17 
30.52 


Detailed  analytical  data  obtained  on  several  samples  of  each  of  the  permitted  colors  (per  cent). 

GREEN   TABLE    NO.  4.     NAPIITIIOL   YELLOW   S. 


Determinations. 


Moisture 

NaCl 

Na  as  NaCl 

Sulphated  ash: 

Al  and  Ee 

Ca 

'h 

S03inNaiS04=Na2S01 

Ratio 

Na  as  Na2So< 

Total  sulphur...'. 

Gutzeit  test 

Heavy  metals  test 

Total  insolubles 

Nonvolatile 

Volatile 

te  ether  extract.. 

Add ■  t 

Total  ether  extract 

Ether  extract  solid 


Serial  Nos. 


23. 


0.70 
6.73 
2.65 

.07 

04 

38.  00 

38.18 

100.3 

12.  32 

8.72 

n.p. 

n.p. 

.05 

..03 

.34 

1.  32 
.062 


o.  28 
3.47 
1.37 

.07 

None. 

48.8 

49.57 

101.6 

15.82 

9.47 

n.p. 

n.p. 

None. 

None. 
.15 
.90 
LOS 

.042 


1.'  .' 
.40 

.07 

None. 

47  1 

47.  32 

100.5 

15.46 

12.  (.3 

n.p. 

n.p. 

None. 

None. 
.14 
.70 
.84 
.04 


0.60 

.61 
.24 

.07 

None. 

5L  4 

51.76 

100.7 

16.68 

12.  42 

n.p. 

n.p. 

None. 

None. 

None. 
.16 
.75 
.91 
.03 


187. 


0.33 
2.86 
1.13 

.28 
None. 

4:'.  44 
100.5 
15.  95 

n.p. 

n.p. 
.05 
None. 
.05 
.10 
.32 


Determinations. 

201. 

209. 

228. 

272. 

280. 

0.5C 

9.31 

.21 
.03 

49.20 
Ml    1 

n.p. 

n.p. 

.  ID 
.  1  1 

.47 

.10 

otao 

1.61 

101.3 

i:  22 

n.p. 

n.  p. 

Ml 

.OCH 

1.13 

.07 

Ml  s 

n.p. 
n.p. 

.  h 

.10 

.80 

.13 

2.  12 
L28 

.07 
N011.'. 

45.  BO 

100.4 
11  78 
10.50 

I'- 
ii.  1-. 

.'.HI 

None. 

u 

.  1  ■ 
.82 
.01 



Bulpl 

\i  and  Fe 

.07 





40   11 



.    ulphur 



£6 

Hea\  \  •                      



Volatile 

in 

Acid  etl                    

Tot  ll  r'll.T  i-.\tr:icl 

EihtT  extract  nlid 

186 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 


Detailed  analytical  data  obtained  on  several  samples  of  each  of  the  permitted  colors  (per 

cent) — Cont  inued . 


GREEN  TABLE  NO.  56.  PONCEAU  3R. 


Determinations. 

Serial 
No.  9. 

Determinations. 

Serial 
No.  9. 

5.76 
19.89 
7.84 

Ratio 

101.20 

NaCl  .. 

Na  as  Na<>S04 

12.36 

Na  as  NaCl 

P- 

n.p. 
.28 

Sulphated  ash: 

Al and  Fe 

|  Heavy  metals  test 

.28 
None. 
38.10 
38.56 

Ca 

.83 

Na2S04 

Total  ether  extract 

1. 11 

S03  in  Na2S04-Na2S04 

Ether  extract  solid 

.326 

GREEN  TABLE  No.  85.  ORANGE  I. 


Determinations. 

Serial  Nos. 

Determinations. 

Serial  Nos. 

16. 

224. 

16. 

224. 

11.06 
8.78 
3.18 

.14 

None. 

30.80 

31.18 

101.3 

9.99 

5.39 
3.51 
1.38 

.07 

.14 

18.00 

18.09 

100.  50 

5.84 

Total  sulphur 

10.12 
P- 
P- 
1.50 
.20 
1.30 
.02 
.20 
.22 
.214 

8.34 

NaCl ...                 

n.p. 

P- 

.55 

Na  as  NaCl. .. 

Sulphate  ash: 

Al and  Fe 

.20 

Ca 

Volatile 

.35 

Na?  SO4     . 

.62 

S03in  Na2S04-NajS04.. 

.20 

Ratio 

Total  ether  extract 

.82 

Na  as  Na2S04 

Ether  extract  solid 

.  254 

GREEN  TABLE  No.  435.  LIGHT  GREEN  SF  YELLOWISH. 


Determinations. 

Serial  Nos. 

57. 

92. 

168. 

233. 

8.32 

.041 
.016 

.70 

3.29 

9.00 

7.78 

86.46 

2.D2 

11.48 

Tr.(p.) 

P- 

.20 

None. 

.20 

.02 

.05 

.07 

.026 

5.08 
.102 
.040 

.28 

.00 

43.40 

43.  96 

101.30 

14.07 

1.-.   11 

Tr.(p.) 

P- 

.45 

.06 

.39 

.02 

.05 

.07 

None. 

5.04 

1.735 

.683 

.14 

.085 

48.00 

46.68 

95.92 

15.  56 

15.  82 

llea\  V. 

P- 

.75 

.60 

.15 

.05 

.05 

.10 

.02 

4.15 

NaCl     

1.530 

Na  as  NaCl 

.603 

Sulphate  ash: 

Al and  Fe 

.14 

Ca    .           

.085 

Na2S04 

S3. 00 

SOt  in  Na2S04—  Na  2S04 

S3.  82 

Ratio  

101.3 

Na  as  Na2SO« 

Total  sul  phur 

17.19 

16.75 

Heavy. 

p. 

Total  Insoluble! 

Nonvolatile .- 

Volatile 

.95 

.60 

.35 

None. 

.  06 

.05 

.02 

ORE  E  N 

TABLE   No 

107.     AM  \l:  Will. 

Determinations. 

Serial  NOS. 

06. 

130. 

162. 

177. 

no. 

1    M 

1      12 

.  It 
.215 
65.20 

6  16 

.07 
.  867 

- 

35.  79 

ll  in 

.  it 
.  03 

60  30 

g  si 

III   (X) 
Us 

is  90 
10.  52 

4.  20 

11.  21 

.  12 
00  00 

61  26 

8.24 

24.21 

v.  M 

Sulphati 

m  and  Fe.. .                         

.21 

.57 

vi  BO 

60.  72 

ANALYSIS   OF   PERMITTED   COLORS,   1907. 


187 


Detailed  analytical  data  obtained  on  several  samples  of  each  of  the  permitted  colors  (per 

cent) — Continued. 

GREEN  TABLE  No.  107.    AMARANTH-Continued. 


Determinations. 


Serial  Nos. 


82. 


Ratio 102. 00 

Na  as  Na2SO< 21. 13 

Total  sulphur :  8. 62 

Copper None. 


Gutzeit  test. 

Heavy  metals  test 

Total  insolubles 

Nonvolatile 

Volatile 

Acetate  ether  extract. 

Acid  ether  extract 

Total  ether  contract.. 
Ether  extract  solid... 


n.p. 

n.p. 

.30 

.12 

.18 

.08 

.07 

.15 


96. 


130. 


162. 


100.80 

17.22 

13.02 

None. 

n.p. 

n.p. 

1.50 

1.10 

.40 

.15 

.15 

.30 

.062 


100.80 

19.39 

8.57 

None. 

n.p. 

n.p. 

2.05 

1.10 

.95 

.18 

.15 

.33 

.052 


101.5 
15.82 
9.42 
.09 
n.p. 
n.p. 
1.05 
.35 
.70 
.20 
.03 
.23 
.040 


177. 


102.1 
19.45 
11.09 

None. 

n.p. 

n.p. 

.90 

.35 

.55 

.02 

.03 

.05 

.044 


219. 


101.9 

16.14 

8.54 

None. 

n.p. 

n.p. 

2.40 

1.15 

1.25 

.30 

.10 

.40 

.054 


GREEN  TABLE  NO.  517.     ERYTIIROSTN. 


Determinations. 

Serial  Nos. 

184. 

200. 

216. 

254. 

9.6 

NaCI  (not  determined) 

Sulphated  a-'h: 

0.14 

None. 

39.00 

39.44 

12.65 

P- 

P- 

.00 

.04 

.50 

.80 

0.14 

None. 

35.  69 

35.44 

11.52 

n.p. 

P- 

.20 

None. 

.20 

.35 

.14 

None. 

31.80 

3246 

10.40 

P- 

P. 

.  66 

.20 

.45 

.10 

0  ">* 

Ca 

NajSO< 

S03  in  NajSO«=NajS04 

Na  as  Na2SO< 

26.  8 

8.56 

Gutzeit  t^st 

P- 

P- 

.90 

Total  insolubles 

Nonvolatile 

.20 

Volatile 

.  70 

Acetate  other  extract 

.  10 

Total  ethrr  extrnrt 

Ether  extract  solid 

.024 

.07 

.02 

.02 

GREEN  TABLE  NO.  692.     INDIGO  DISULPIIO  ACID. 


Doterminations. 

Serial  Nos. 

Determinations. 

Serial  No*. 

90. 

195. 

249. 

90. 

l".-,. 

249. 

Moisture 

7.25 
7.08 

2.77 

.42 
2m.  74 

5.32 
11.26 

.14 
55.40 

17.  '7 

7.31 
7.02 
2.  77 

.71 
102  B 

Total  sulphur 

10.30 
P  (?) 

LOB 
.09 

.07 
.008 

.80 

.if.' 
.10 
,U 
.OH 

10m 

V.i  l. 

1.  15 

\;i('l 

Sulphated  ash: 

Heavy  metals  tost 

Total  Insoluble*  

\i  a  1  Pe 

- 



Acetate  eth<  • 

\ciii  ether  extract 

1  ol  il  ether  • 

Ether  <                 1 

n> 



In    NaiSO«=Na, 

I     

.01 



RECALCULATION    OF    ANALYTICAL    DATA   ON    BASIS   <»l"   COLORING 
KATTEB    PRESENT. 

The  difficulties  in  the  way  of  translating  these  analytical  data  into 
proximate  constituents  are  so  great,  in  bo  many  of  the  cases,  i 
make  any  attempts  to  obtain  practical  results  in  thai  way  absolutely 


188 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


useless;  the  amount  of  material  on  hand  was  unfortunately  so  small 
at  the  beginning  (2  ounces  or  less,  in  most  instances)  that  the  utmost 
economy  of  material  was  necessary  to  get  the  data  reported,  on 
account  of  the  large  amount  of  material  needed  in  the  exploratory 
work  done  in  trying  out  the  methods  for  determining  arsenic,  heavy 
metals,  and  ether  extractives. 

In  the  arsenic  test  the  coloring  matter,  as  a  whole,  was  considered, 
and  no  attempt  was  made  to  get  at  the  actual  amount  of  real  coloring 
matter  in  the  exact  weights  of  the  material  as  a  whole,  used  for  such 
examination,  and  consequently  the  results  are  not  translatable  into 
actual  weights  of  real  color  used.  It  is  obvious  that  if  2  grams,  or 
other  weight  of  the  substance  as  a  whole,  failed  to  pass  any  test  when 
the  whole  amount  was  considered  as  though  it  were  all  color,  the 
material  could  not  possibly  have  passed  those  tests  if  amounts  thereof, 
corresponding  to  the  prescribed  weights  of  actual  color  used,  were 
taken;  also  it  is  clear  that  if  the  sample,  as  a  whole,  passed  a  given 
test,  at  a  given  weight  thereof,  it  would  not  necessarily  have  passed 
that  test  had  an  amount  thereof,  corresponding  to  that  same  weight 
of  actual  color,  been  used. 

The  amount  of  actual  or  real  coloring  matter  in  27  of  these  30 
specimens  is  not  greater  than  shown  in  the  following: 

Per  cent  of  actual  coloring  matter  in  27  samples. 


Name  of  color. 


Serial 
No. 


Percent. 


Serial 
No. 


Per  cent. 


Naphthol  Yellow  S 

Ponceau  3R 

Orange  I 

Amaranth 

Light  Green  SF  Yellowish 

Erythrosin 

Indigo  Disulpho  Acid 


23 
73 

108 

142 

187 

9 

16 

82 

90 

130 

57 

92 

210 

90 

195 


91.20 
95.20 
97.80 
97.88 
90.34 
73.24 
78.44 
50.40 
78.95 
55.00 
91.37 
94.30 
89.05 
84.11 
05.10 


201 
209 
228 
272 
280 


75.56 
93.19 
95.  72 
92.81 

79.  47 


224 

89.  n 

162 

63.52 

177 

66.  40 

219 

64.26 

168 

92. 37 

233 

93.32 

249 

84.47 

In  order  to  make  these  analytical  results  comparable  among  them- 
selves and  with  other  analytical  results  later  to  be  given,  the  items 
common  salt,  volatile  and  nonvolatile  insolubles,  total  insolubles, 
acetate  ether  extract,  acid  ether  extract,  and  total  ether  extract  of 
the  preceding  tabulations  have  been  recalculated  in  parts  per  100 
of  actual  or  real  coloring  matter  as  just  enumerated: 


ANALYSIS   OF   PERMITTED   COLORS,    190^ 


189 


Analytical  data  recalculated  to  parts  per  hundred  of  coloring  matter  present. 
GREEN  TABLE  NO.  4.    NAPHTHOL  YELLOW  S. 


Determinations. 

Serial  Nos. 

23. 

73. 

108. 

142. 

IS, 

201. 

209. 

228. 

272. 

280. 

Common  salt 

7.38 

3.64 

1.04 

0.62 

2.97 

31.53 

4.38 

2.99 

3.51 

11.82 

Insolubles: 

Volatile 

.02 
.03 

.00 
.00 

.00 
.00 

.00 
.00 

.05 
.00 

.13 
.27 

.86 
.00 

.02 
.10 

.97 
.00 

1.46 

.05 

Total 

.05 

.00 

.00 

.00 

.05 

.40 

.86 

.12 

.97 

1.51 

Ether  e-v- tract: 

.37 
1.07 

.16 
.95 

.14 
.72 

.16 
.77 

.10 
.33 

.19 
.44 

.27 
1.16 

.08 
.94 

.16 

.78 

.13 

.97 

Total 

1.44 

1.11 

.86 

.93 

.43 

.63 

1.43 

1.02 

.94 

1.10 

GREEN  TABLE  NO.  56.  PONCEAU  3R. 


Determinations. 

Serial  No. 
9. 

Determinations. 

Serial  No. 
9. 

27.16 

Ether  ex  tract  : 

Acetate 

0.38 

Volatile 

Acid 

1.13 

Total 

1.51 

GREEN  TABLE  NO.  85.  ORANGE  I. 


Determinations. 


Common  salt. 


Insoluble: 

\  "lutile 

Nonvolatile. 

Total 


Serial  Nos. 

16. 

224. 

11.19 

3.91 

1.66 

.  25 

.39 
.23 

1.91 

.62 

Determinations. 


Ether  extract: 
Acetate. . . 
Acid 


Total. 


Serial  Nos. 


In. 


0.02 
.25 


.27 


224. 


0.69 
.23 


.92 


GREEN  TABLE  NO.  107.    AMARANTH. 


Determinations. 

Serial  Nos. 

82, 

96. 

130. 

162. 

177. 

219. 

84.87 

39.97 

42.85 

37  39 

1 

Volatile  

.21 

.51 

1      1 

1.71 

1.10 

1  93 

1  78 

Tot:il 

.53 

1.90 

3.69 

1.65 

1.37 

3  71 

Ether  extract: 

.11 
.12 

.19 
.19 

,1? 

.31 

.03 

46 

And 

15 

Total 

.26 

.38 

.59 

.36 

.08 

61 

190 


COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 


Analytical  data  recalculated  to  parts  per  hundred  of  coloring  matter  present — Continued. 

GREEN  TABLE  NO.  435.    LIGHT  GREEN  SF  YELLOWISH. 


Determinations. 

Serial  Nos. 

57. 

92. 

168. 

232. 

0.04 

0.10 

1.88 

1  04 

Insoluble: 

Volatile 

.22 
.00 

.41 

.00 

.16 
.65 

.38 

Nonvolatile 

.64 

Total 

.22 

.47 

.81 

1.02 

Ether  extract: 

Acetate 

.02 
.05 

.02 
.05 

.05 
.05 

.05 

Acid 

05 

Total 

.07 

.07 

.10 

.10 

GREEN  TABLE  NO.  517.    ERYTHROSIN. 


Determinations. 

Serial 
No.  216. 

Determinations. 

Serial 
No.  216. 

Common  salt 

Ether  extract: 

0  11 

Insoluble: 

0.50 
.22 

Acid 

Total 

N  onvolatile 

.11 

Total 

.72 

GREEN   TABLE 

NO.  692. 

INDIGO   SULPHO  ACID. 

Determinations. 

Serial  Nos. 

Determinations. 

Serial  Nos. 

90. 

195. 

249. 
8.  31 

90. 

195. 

249. 

Common  salt 

44.02 

Ether  extract: 

0.02 
.06 

0.03 
.15 

0  02 

1.25 

.  59 

1.23 

.00 

.77 
.59 

Acid 

.04 

Total 

.08 

.18 

Total 

1.84 

1.23 

1.36 

MARKET  QUALITY  OF  THE  SEVEN  PERMITTED  COLORS. 

That  the  quality  of  the  lots  of  the  seven  permitted  colors  of  Food 
Inspection  Decision  No.  70  offered  on  the  markets  of  the  world  after 
the  issuance  of  that  decision  was  no  heller  than  that  of  the  lots  just 
reported,  if  as  good,  appears  from  the  paper  of  E.  G.  Kohnstamm  enti- 
tled, "Certified  Food  Colors:  The  Difficulties  in  the  Way  of  their 
Manufacture/5  presented  to  the  Seventh  International  Congrec 
Applied  Chemistry  held  in  London,  May  and  dune,  1909,  and  pub- 
lished in  abstract  form.     This  abstract  reads  .-is  follows: 

The  coal-tar  colors  permitted  under  the  food  and  drugs  act  of  the  United  States  ar< 
in  Dumber,  which  must  be  is  a  high  state  of  purity.    The  author  slates  thai 
of  the  colors  on  the  markets  of  the  vrorld,  at  the  time  oi  testing,  would  meet  these 
requirements. 


ANALYSIS- OF   PERMITTED   COLORS,   1907.  191 

Of  these  seven  colors,  189  samples,  from  every  possible  source,  and  representing  all 
the  leading  manufacturers,  are  here  reported  on,  and  the  results  of  their  examina- 
tion reasonably  establish  the  necessity  of  food  color  certification.  Of  these  189  sam- 
ples, the  worst  were  offered  for  food  coloring  purposes  and  seemed  to  be  so  offered 
because  unfit  for  any  other  purpose. 

Naphthol  Yellow  S. — Sixty-four  samples  examined,  ranging  in  shade  from  clear 
bright  yellow  to  a  dirty  brownish  or  green  color.  All  contained  Martius  Yellow,  some 
more  than  1  per  cent  thereof;  some  contained  as  high  as  2  per  cent  and  even  3  per  cent 
unconverted  initial  material  or  decomposition  products.  Forty-one  contained  exces- 
sive arsenic  and  29  excessive  heavy  metals. 

Orange  I. — Twenty-eight  samples  examined;  all  contained  decomposition  products 
varying  from  a  slight  amount  to  over  50  per  cent;  free  <r-naphthol  was  found  in  most 
samples;  in  12  it  was  as  high  as  2  per  cent;  insoluble  matters  were  as  high  a^  1  per  cent ; 
lead  to  the  extent  of  0.5  per  cent  was  found  in  one  sample;  shading  by  dded  colors 
and  excessive  amounts  of  arsenic;  lead  and  iron  were  frequent. 

Amaranth. — Thirty-eight  samples  examined;  none  were  pure,  and  all  contained 
arsenic  in  excessive  amounts,  and  in  one  case  as  high  as  0.1  per  cent;  all  contained 
added  color,  principally  an  acid-violet.  Iron  as  high  as  0.1  per  cent;  insoluble  matter 
as  high  as  1£  per  cent;  was  most  heavily  loaded  with  salt  of  all  seven  colors. 

Ponceau  3R. — Thirty-six  samples  examined;  the  purest  of  all  colors  tested;  not 
toned;  heavily  loaded  with  salt;  much  insoluble  matter  was  present;  decomposition 
products  were  absent;  iron,  0.01  per  cent;  12  contained  excessive  amounts  of  arsenic 
and  14  contained  excessive  amounts  of  heavy  metals. 

Erythrosin. — Twelve  samples  examined;  10  were  not  erythrosin  at  all ;  of  the  other 
two,  one  was  low  in  iodin  and  one  contained  arsenic. 

Light  Green  S  F  Yellowish. — Thirteen  samples  examined;  only  one  free  from 
arsenic;  nine  contained  lead  or  copper;  one  contained  manganese;  none  were  1<  . 

Indigo  Disulphonic  Acid. — Eight  samples  examined;  none  were  pure;  the  iron  con- 
tent was  as  high  as  1.5  percent;  all  were  loaded  with  salt  or  Glauber's  salt.     On 
tained  excessive  amount  of  arsenic  and  two  excessive  amounts  of  heavy  metal.-. 

The  difficulties  consist  in  keeping  the  undesirable  materials  out  of  the  dyes  or  in 
separating  them  from  the  crude  dyes,  or  both. 

In  this  connection  the  following  statement  made  by  Dr.  E.  Ludwig, 
of  Vienna,  at  the  International  Congress  of  Medicine  held  in  Buda- 
pest, August,  1909,  may  be  of  interest: 

The  author,  at  an  order  of  a  court,  at  the  beginning  of  the  seventies  in  the  last  cen- 
tury, examined  approximately  200  samples  of  food  products  confiscated  as  suspicions 
and  taken  from   numeroi.  of  a   then  suburb  of  Vienna;  these  Sample! 

included  solid  confectionery,  fruit  sirups,  spirits,  etc.  Be  found  that  more  than 
90  per  cent  of  these  things  were  colored  with  magenta  and  contained  arsenic.  In  some 
of  ill-  the  preparation  used  for  coloring,  the  so-called  "couleur, 

found,  which  proved  to  be  a  solution  of  magenta  and  in  which  there  were  contained  8 
per  cent  of  arsenic  in  the  form  of  arsenous  acid  and  of  ai  id.    According  to  th< 

statements  of  a  qualified  dyestuff  maker,  this  ■•couleur"  was  a  mother  liquor 

ita  manufacture,  which  was  very  difficultly  saleable  and  which,  however,  a 
1  talked  onto  Ignorant  producers  of  and  dealers  in  foods. 

Schacherl  (p.  XOJfi)  says:  "It  Bhould  be  required  of  all  permitted 
coloring  matters  that  they  .shall  not  contain  substances  which  arc 
harmful  to  health,  <>r  even  suspicious,  cither  in  chemical  union  • 
contaminations."  The  following  page*  Section  XV)  sbxw  how 
closely  this  requirement  has  been  met  aa  a  result  of  quality  control 
on  the  part  of  the  Department  of  Agriculture. 


192  J  -TAB  COLORS  USED  IN  POOD  PRODUCTS. 

XV.  GUIDES   IN  DETEMUNIXG  DEGREE    OF    PUEITY   AND 

CLEANLINESS. 

In  view  of  the  absence  of  any  statements  in  the  literature  defining 
the  purity  of  the  colors  physiologically  examined  with  such  accuracy 
that  another  could  obtain  with  reasonable  certainty  the  same  degree 
of  cleanliness,  it  became  necessary  to  devise  some  guide,  no  matter 
how  empirical,  in  the  setting  up  of  standards,  tentative  or  otherwise. 

As  a  first  consideration  it  was  held  that,  in  view  of  the  fact  that  all 
of  the  physiological  work  had  been  done  with  specimens  of  coal-tar 
colors  of  commercial  purity,  it  would  be  reasonable  to  suppose  that 
coal-tar  colors  produced  in  the  purest  form  possible  with  present-day 
methods  would  certainly  be  as  clean  and  as  free  from  admixture  as 
any  of  the  commercial  products  subjected  to  physiological  test.  It 
•lonsidered  unreasonable  to  expect  that  increasing  the  degree  of 
purity  of  these  substances  could  in  any  way  increase  any  harmful 
property  possessed  by  them.  Certainly  in  the  case  of  Xaphthol 
Yellows,  where  Martius  Yellow  is  a  usual  contaminant,  it  can  hardly 
be  maintained  that  decreasing  the  amount  of  Martius  Yellow  would 
increase  any  harmful  property  which  might  reside  in  Xaphthol  Yel- 
low S  proper:  in  the  case  of  Ponceau  3  R  it  could  hardly  be  argued 
that  any  undisazotized  base  or  decomposition  products  of  diazo 
compounds  tended  to  correct  or  counteract  any  harmful  property 
that  might  reside  in  Ponceau  3  R  proper;  nor  could  it  be  maintained 
that  Orange  I  free  from  uncombined  alpha-naphthol  was  more  harmful 
than  Orange  I,  contaminated  with  alpha-naphthol,  and  so  on  through 
the  list  of  the  seven  permitted  colors.  This  point  would  not  be 
raised  had  it  not  been  pressed  repeatedly  by  different  persons  as  a 
serious  objection  to  quality  control  and  purity  standards  of  the  seven 
permitted  colors  of  Food  Inspection  Decision  No.  76. 

With  this  rule  in  mind,  and  referring  to  the  tabulated  results  of  the 
analyses  of  the  30  specimens  of  the  seven  permitted  colors  just  given, 
the   items   in    the    analytical   statements   will   each   be   separately 
1. 

Common  salt  and  ether  extractive. — Common  salt  is  a  legitimate  com- 
ponent of  commercial  brands  of  coal-tar  colors  in  so  far  as  I 
coal-tar  colors  are  obtained  by  the  so-called  "salting  out"  process. 
The  coal-tar  colors  are  recovered  from  solution  by  the  addition  of 
common  salt,  which  has  the  peculiar  property  of  separating  the  coal- 
i  olor  from  the  water  solution  as  an  undissolved  solid.  The 
-^ar  color  so  obtained  will  contain  more  or  less  salt,  which,  from  a 
commercial  manufacturing  point  of  1  <fore  an  unavoidable 

Mtuent.     The    amount    of   salt   so    accompanying    the   coal-tar 
color  depends  upon  the  amount  added  to  the  color  solution,  and  this 

■  i  chaustion  of  the  coal-tar  color  solution 
is  attempted,     it  ia  a  matter  of  common  experience  that,  as  a  rule, 


GUIDES  IX  DETERMINING  PURITY.  193 

the  coal-tar  color  first  separating  in  the  salting-out  process  is  cleaner 
and  less  contaminated  than  the  portions  last  separating.  In  an 
endeavor  to  recover  as  far  as  possible  all  the  dissolved  coal-tar 
coloring  matter  the  manufacturer  adds  a  large  excess  of  salt,  and 
this  carries  with  it  a  large  amount  of  organic  matter  not  coloring 
matter,  as  can  be  seen  from  the  preceding  analyses,  where  a  high 
salt  content  is  almost  always  accompanied  by  a  high  ether  e.\ 
content.  The  ether  extract  content  is  a  measure  of  the 
organic  impurities  of  the  coloring  matter. 

The  objection  to  an  excessive  amount  of  salt  in  coal-tar  coloring 
matters,  when  they  are  to  be  used  for  food-coloring  purpo- 
not  reside  in  the  salt  per  se,  but  is  due  to  the  fact  that  .    salt 

content  seems  generally   to   be   accompanied   by   an   unnecessarily 
large  amount  of  organic  material  not  coloring  matter,  and  nothing 
good  is  known  of  such  material,  which  is  more  than  likely  ( 
harmful. 

The  acetate  ether  extract  is  supposed  to  represent  that  part  of  the 
organic  material  not  coloring  matter  whi  only  slightly, 

basic  properties;   the  acid  ether  extract  is  su]  to  represent 

part  of  the  organic  material  not  coloring  matter  which  has  acid 
properties.     In  the  case  of  Xaphthol  Yellow  S  the  acid  ether  ex 
will  contain  all  of  the  Martuis  Yellow,  and  very  likely  will  c 
substantially  of  it.     In  the  case  of  Erythrosin.  of  course,  no  acid  ether 
extraction  was    attempted    because    the    color    I  f   ether- 

soluble. 

The  follow;  lation  shows  the  percentages  of  salt  1 

the  amount  of  coloring  matter  pres  26 of  the*         mens 

before  reported   on,   arranged   v  n   permi 

colo 

Xaphthol  Yellow  8:   0.62;   1.04;  2.97;  5; 

^e,  6.99.) 
Ponceau  3  R:    27.16. 
Orange  I:    3.91;  11.19.     ('Avcnu 
■ranth:  1-   . 

I 
Indigo  Disulpho  Arid 

The  follow':  vo  the  £ 

xtract: 

•T. 

btholYeU 

Orai 

Ain.irv.!:- 

il°— Boll.  147—12— 


194         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

Light  Green  SF  Yellowish:  0.02;  0.02;  0.05;  0.05.     (Average,  0.035.) 

Erythrosine:  0.11. 

Indigo  Disulpho  Acid:  0.02;  0.02;  0.03.     (Average,  0.03.) 

ACID    ETHER   EXTRACT. 

Naphthol  Yellow  S:  0.33;  0.44;  0.72:  0.77:  0.78;  0.94;  0.95;  0.97;  1.07;  1.16.     (Aver- 
age, 0.81.) 

Ponceau  3R:  1.13. 

Orange  I:  0.23;  0.25.     (Average,  0.24.) 

Amaranth:  0.05;  0.05;  0.12;  0.15;  0.19;  0.27.     (Average,  0.14.) 

Light  Green  SF  Yellowish:  0.05;  0.05;  0.05;  0.05.     (Average,  0.05.) 

Indigo  Disulpho  Acid:  0.04;  0.06;  0.15.     (Average,  0.0S.^ 

TOTAL    ETHER    EXTRACT. 

Naphthol  Yellow  S:  0.43;  0.63;  0.86;  0.93;  0.94;  1.02;  1.10;  1.11;  1.43;  144.     (Aver- 
age, 0.99.) 

Ponceau  3R:  1.51. 

Orange  I:  0.27;  0.92.     (Average,  0.59.) 

Amaranth:  0.08;  0.26;  0.36;  0.38;  0.59;  0.61.     (Average,  0.38.) 

Light  Green  SF  Yellowish:  0.07;  0.07;  0.10;  0.10.     (Average,  0.09.) 

Erythrosin:  0.11. 

Indigo  Disulpho  Acid:  0.06;  0.08;  0.18.     (Average,  0.11.) 

Insoluble  matter. — The  amount  of  insoluble  matter  (total,  volatile, 
and  nonvolatile)  is  a  measure  of  the  cleanliness  of  the  materials 
used,  as  well  as  of  the  cleanliness  of  treatment  during  the  manu- 
facture of  the  coloring  matter.  The  following  tabulation  shows  the 
variations  in  these  three  figures  for  each  of  the  26  specimens  of  the 
7  permitted  colors,  examined,  as  in  the  preceding  cases: 

Insoluble  matter. 

VOLATILE    INSOLUBLE. 

Naphthol  Yellow  S:  0.00;  0.00;  0.00;  0.02;  0.02;  0.05;  0.13;  0.86;  0.97;  1.46.     (Aver- 
age, 0.35.) 

Orange  I:  0.39;  1.66.     (Average,  1.03.) 

Amaranth:  0.32;  0.51;  0.83;  1.10;  1.71;  1.93.     (Average,  1.07.) 

Light  Green  SF  Yellowish:  0.16;  0.38;  0.22;  0.41.     (Average,  0.29.) 

Erythrosin:  0.50. 

Indigo  Disulpho  Acid:  0.77;  1.23;  1.25.     (Average,  1.08.) 

NONVOLATILE    INSOLUBLE. 

Naphthol  Yellow  S:  0.00;  0.00;  0.00;  0.00;  0.00;  0.00;  0.03;  0.05;  0.10;  0.27.     (Aver- 
age, 0.05.) 

Orange  I:  0.23;  0.25.     (Average,  0.24.) 

Amaranth:  0.21;  0.54;  0.55;  1.39;  1.78;  1.98;    (Average,  1.08.) 

Light  Green  SF  Yellowish:  0.00;  0.06;  0.64;  0.65.     (Average,  0.34.) 

Erythrosin:  0.22. 

Indigo  Disulpho  Acid:  0.00;  0.59;  0.59.     (Average,  0.36.) 

TOTAL   INSOLUBLE. 

Naphthol  Yellow  S:  0.00;  0.00;  0.00;  0.05;  0.05;  0.12;  0.40;  0.86;  0.97;  1.51.  (Aver- 
age, 0.40.) 

Orange  I:  0.62;  1.91.     (Average,  1.27.) 


GUIDES   IN   DETERMINING   PURITY.  195 

Amaranth:  0.53;  1.37;  1.65;  1.90;  3.69;  3.71.     (Average,  2.14.) 
Light  Green  SF  Yellowish:  0.22;  0.47;  0.81;  1.02.     (Average.  0.63.) 
Erythrosin:  0.72. 
Indigo  Disulpho  Acid:  1.23;  1.36;  1.84.     (Average,  1.48.) 

Work  subsequent  to  these  analyses  showed  that  the  insoluble 
matter,  particularly  the  nonvolatile  insoluble  matter,  was  greater 
in  certain  batches  than  in  others,  and  that  these  amounts  were  in 
excess  of  the  maximum  amounts  reported  therefor.  Examination 
showed  that  these  increased  amounts  of  insoluble  matter  were 
probably  due  to  variations  in  the  water  delivered  to  the  factories 
by  their  respective  municipal  water  supplies,  since  it  was  noted  that 
in  two  or  more  cases  the  batches  containing  an  exceptionally  large 
amount  of  nonvolatile  insoluble  matter  were  manufactured  at  a 
time  when  the  city  water  supply  was  abnormally  hard;  this  item, 
therefore,  has  been  made  in  some  instances  a  little  more  elastic  than 
the  preceding  analyses  would  seem  to  justify. 

Arsenic. — Examination  of  the  preceding  tabulations  shows  that 
14  out  of  30  specimens  tested  passed  the  Gutzeit  test  for  arsenic,  and 
16  failed  to  pass. 

Heavy  metals. — Inspection  of  the  preceding  tables  shows  that  13 
out  of  30  specimens  passed  this  test,  and  that  17  failed  to  pass. 

Combined  arsenic  and  heavy  metals  test. — Inspection  of  the  preceding 
tables  shows  that  11  out  of  30  passed  both  tests  jointly;  that  3 
passed  the  arsenic  test  and  failed  to  pass  the  heavy  metals  test;  and 
that  2  passed  the  heavy  metals  test  and  failed  to  pass  the  arsenic 
test. 

Moisture. — The  amount  of  moisture,  as  inspection  of  the  preceding 
analyses  shows,  is  variable,  and  is  a  factor  not  under  easy  control. 
As  long  as  the  coloring  matters  submitted  for  foundation  certification 
were  in  powder  form  and  the  analyses  disclosed  the  actual  percentage 
of  coloring  matter  it  was  considered  that  any  control  of  this  item 
would  involve  an  amount  of  labor  and  provide  opportunities  for 
friction  wholly  out  of  proportion  to  any  benefit  that  at  present  could 
be  realized  therefrom.  Therefore  such  control  was  not  instituted, 
although  it  by  no  means  follows  that  the  time  may  not  come  when 
control  of  this  item  will  be  necessary. 

Sulphur  and  sulyhated  ash.—  These  two  determinations  in  the 
case  of  all  the  permitted  colors,  except  Erythrosin,  give  a.  rough 
measure  of  the  extent  of  the  sulphonation  and  of  the  saturation  of 
the  sulphonic  acids  with  sodium.  It  is  not  the  function  of  these 
two  items  to  exclude  the  isomeric  modifications,  nor  was  any  test 
applied  to  such  of  these  30  specimens  as  were  examined  in  this  respect 
to  determine  the  presence  or  absence  of  such  products.  The  attempts 
made  in  this  direction  are  of  a  later  date  than  the  analyses  already 
reported,  and  are  indicated  on  page  210  of  this  report. 


196         COAL-TAR  COLOES  USED  IX  FOOD  PRODUCTS. 

With  these  data  available,  and  with  the  general  rule  stated  at  the 
opening  of  this  section  in  mind,  it  was  regarded  as  the  proper  course, 
when  determining  upon  standards,  to  require  that  each  color  should 
pass  the  combined  heavy  metals  and  arsenic  test  of  the  United  States 
Pharmacopoeia,  and  in  other  respects  should  be  as  clean  and  as  high- 
grade  as  the  best  of  each  class  given  in  the  preceding  analyses.  Just 
how  closely  it  was  possible  to  adhere  to  this  ride  will  be  shown 
later. 

With  respect  to  the  arsenic  requirement,  there  has  been  a  great 
deal  of  discussion  brought  on  by  those  interested  in  the  manufacture 
of  these  colors.  It  was  protested  that  colors  could  not  be  made 
uniformly  and  continuously  under  manufacturing  conditions,  which 
would  contain  an  amount  of  arsenic  so  small  that  a  quantity  of  the 
product  containing  2  grams  of  the  coloring  matter  in  question  would 
not  respond  to  the  Gutzeit  test  in  the  United  States  Pharmacopoeia. 
The  results  above  given  with  respect  to  conformity  or  nonconformity 
to  the  Gutzeit  test,  were,  with  a  great  deal  of  justification,  not  regarded 
as  conclusive,  because,  as  has  been  previously  stated,  there  was  no 
certainty  that  the  amount  of  coloring  matter  actually  taken  did 
represent  2  grams.  Tn  view  of  the  fact  that  the  United  States  Phar- 
macopoeia prescribes  for  the  only  coal-tar  color  in  it,  namely,  Methy- 
lene Blue,  that  it  shall  be  so  free  from  arsenic  that  2  grams  fail  to 
respond  to  the  Gutzeit  test,  it  was  considered  perfectly  justifiable 
to  adhere  to  that  requirement  until  it  could  be  conclusively  shown 
that  it  was  unreasonable  and  incapable  of  attainment.  Results 
described  in  the  pages  that  follow  show  that  it  has  been  possible  to 
make  all  the  7  permitted  colors  of  Food  Inspection  Decision  No.  76 
so  free  from  arsenic  that  the}T  comply  with  (he  Pharmacopoeia] 
test. 

With  respect  to  the  heavy  metals,  no  deviation  was  necessary  for 
the  nonferrous  metals  from  the  test  of  the  Pharmacopoeia;  for  iron, 
however,  it  was  found  necessary  to  increase  the  limit  to  substantially 
0.005  part  per  100  of  actual  coloring  matter.  The  reason  for  this  is 
that  at  one  time  or  another  all  of  the  seven  permitted  coloring  matters 
in  the  course  of  their  manufacture  come  in  contact,  with,  or  are  con- 
tained in,  vessels  of  iron,  and  it,  seems  t<>  be  almost  impossible  to 
keep  iron  out  to  an  extent  which  would  bring  the  color  within  the 
pharmacopoeia!  test.  It  has  been  shown  that  there  were  1:5  colors 
(.n  the  market  in  1907  which  contained  so  little  iron  that,  they  failed 
to  respond  to  the  heavy  metals  test  of  the  Pharmacopoeia  in  that 

respect;  but  here  again  the  same  criticism  holds  good  as  in  the  arsenic 
I  hat  there  is  no  certainty  that  the  amounts  taken  for  the  heavy 

metals  tests  were  equivalent  in  each  ca.se  to  1  grain  of  actual  coloring 

matter,  and  subsequent  experience  seems  to  confirm  the  correctness 


GUIDES   IN   DETERMINING   PURITY.  197 

of  that  criticism;  therefore  the  rule  for  cleanliness  of  product,  as  just 
given,  has  been  modified  in  that  respect  and  to  that  extent. 

That  it  was  only  fair  and  reasonable  to  expect  considerable 
improvement  in  the  cleanliness  and  purity  of  food  colors  was  made 
evident  by  an  examination  of  two  substances  sold  in  the  United 
States  in  large  quantities  for  the  purpose  of  making  a  very  cheap 
red  coal-tar  coloring  matter,  which  is  used  in  many  of  the  cheapest 
coloring  operations,  for  paints,  inks,  etc.  These  substances  are 
paranitranilin  and  betanaphthol.  They  were  found  in  the  United 
States  market  in  such  a  condition  of  cleanliness  and  purity  that  had 
they  been  suitable  for  use  in  foods  no  objection  could  be  raised 
against  them  on  these  scores.  They  complied  with  the  requirements 
of  the  United  States  Pharmacopoeia  with  respect  to  freedom  from 
arsenic  and  all  heavy  metals,  inclusive  of  iron.  The  significance  of 
this  lies  in  the  fact  that  all  the  raw  materials  entering  into  the  manu- 
facture of  paranitranilin  and  betanaphthol  also  enter  into  the  manu- 
facture of  the  seven  permitted  colors  of  Food  Inspection  Decision 
No.  76,  and  that  the  only  source  of  arsenic  in  food  colors,  and  probably 
the  only  way  in  which  iron  could  be  introduced  into  them,  is  by  way 
of  the  materials  entering  into  the  manufacture  of  paranitranilin 
and  betanaphthol,  and  since  it  has  been  shown  to  be  commercially 
possible  to  keep  those  bodies  out  of  paranitranilin  and  betanaphthol, 
and  since  there  is  no  occasion  whatever  for  arsenic  or  iron  or  other 
heavy  metal  being  present  in  any  of  the  materials  used  in  the  manu- 
facture of  the  seven  permitted  colors  of  Food  Inspection  Decision 
Xo.  76,  over  and  above  the  materials  used  in  the  manufacture  of  para- 
nitranilin and  betanaphthol,  there  was  every  reason  for  believing 
that  the  seven  permitted  colors  of  Food  Inspection  Decision  No.  70 
could  ultimately  be  manufactured  and  marketed  in  the  same  degree 
of  cleanliness  and  purity  that  paranitranilin  and  betanaphthol  are 
marketed;  in  oilier  words,  that  food  colors  could  be  made  as  clean 
and  as  pure  as  paint  colors,  a,  condition  not  existing  in  the  food-color 
market  of  the  United  States  in  the  summer  of  L907. 

The  results  of  the  control  exercised  by  the  Department  of  Agricul- 
ture over  the  quality  of  food  colors,  as  compiled  in  the  following 
section,  fully  justify  such  expectations,  as  well  as  the  aim  to  make 
coal-tar  colors  when  used  for  food  purposes  of  the  same  high  degree 
of  cleanliness  and  purity  as  when  they  are  to  he  used  a-  drugs  or  as 
they  actually  are  when  used  for  the  man u fact  \i re  of  paints  and  printer's 
inks;  that  is  to  say,  that  the  coal-tar  color  used  in  a  colored  food 
should  be  as  clean  ;i-  the  coal-tar  color  used  in  making  t  he  ink  on  t  he 

label  of  Mich  colored  food,  the  very  reverse  of  the  .situation  existing 
prior  to  the  quality  control  now  established 


198 


COAL-TAR    COLORS   L'SED   IX    FOOD   PRODUCTS. 


XVI.  ANALYSES   OF  CERTIFIED  LOTS   OF  PERMITTED   COLORS, 

1909-10. 


TABULATION  OF  RESULTS. 

The  analytical  results  obtained  on  74  batches  of  certified  colors, 
totaling  upward  of  32,000  pounds,  are  given  in  the  following  tables. 
The  analytical  results  are  the  work  of  the  New  York  Food  and  Drug 
Inspection  Laboratory  in  the  course  of  checking  up  the  analytical 
results  certified  to  in  foundation  and  in  supplementary  certificates. 
The  period  covered  by  these  examinations  is  approximately  from 
July,  1909,  to  January  1,  1910. 

Naphthol  Yellow  S. 

[Figures  calculated  to  100  parts  pure  color  and  arranged  in  the  order  of  their  size.  Figures  on  the  same 
horizontal  lines  do  not  refer  to  the  same  samples;  the  dash  line  shows  the  location  of  the  average  of  each 
column.] 


Insolubles. 

Ether  extractives. 

Com- 
mon 
salt. 

Sul- 
phur. 

So- 
dium. 

Cal- 
cium. 

Number  of  batches. 

Total. 

Inor- 
ganic. 

Neu- 
tral. 

Alkali. 

Lcid. 

Total. 

1 

2     

0.170 
.130 

.097 
.090 

.082 

.079 

0.100 
.078 

.050 
.040 

0.036 
.026 

.024 
.023 

.019 

.018 

0.016 
.007 

.006 
.006 

.005 

.005 

0.067 
.065 

.042 
.038 

.036 

0.088 
.073 

.072 
.064 

.061 

.057 

.056 
.054 

4.06 
2.26 

1.68 
1.41 

1.30 

9.23 
8.99 

8.98 
8.90 

8.89 

13.27 
13.21 

0.13 
.13 

3     

12.92 
12.90 

12.89 

12.89 

12.87 
12.87 

12.81 
12.75 

.05 

4           

.04 

5 

.040 

.030 

.032 
.030 

.010 
.010 

G 

.034 

.031 
.026 

.025 
.025 
.020 
.018 

.63 

.03 

.48 

.47 
.  26 

.24 
.19 
.19 

S.86 
8.85 

8.71 
8.70 
8.62 

7  

.070 
.000 

.055 
.050 
.0.50 
.030 
.030 

.016 
.012 

.011 
.010 
.007 
.006 

.004 
.004 

.000 
.000 
.000 
.000 

8  

9  

.048 
.045 
.045 
.045 
.044 

10 

11     .           

12                        

13 

Average 

Above 

Below 

.076 
ti 
7 

.043 
4 
0 

.017 
6 
6 

.004 

6 
6 

.035 
5 

7 

.051 
8 
5 

1.06 

."> 
8 

8.87 
5 

ti 

12.93 
2 
8 

.09 
2 
2 

Ponceau  .,/,'. 

[Figures  calculated  to  KM)  parts  pure  color  and  arranged  in  Hie  order  of  their  size.  Figures  in  the  same 
horizontal  line  do  not  refer  to  the  same  sample;  Che  dash  line  shows  the  location  of  the  average  of  each 
column.] 


Number  of 
batches. 

Insoluble. 

Fther  extractives. 

Com- 
mon 

salt. 

So- 
dium 

sul- 
phate. 

Sul- 
phur. 

So- 
dium. 

(V.l- 
cium. 

Boiling 
point  of 
cumi- 

din. 

Total. 

Inor- 
ganic. 

Neu- 
tral. 

Alkali. 

Acid. 

Total. 

1 

2 

0.56 
.43 

.41 

.27 

0.29 
.20 

.17 

0.166 
.163 

.  L61 

0.034 

.033 

.  032 

0.019 

.ills 

.ills 

.018 

.017 

.017 
.016 
.014 

0.216 
.218 

.  201 

:..  73 
6.87 

0.06 
.06 

12.96 

9.61 

9.81 
9.81 

9. 28 

0.18 
.18 

222-236 
222-236 

3 

.00 
.00 

.(HI 

.no 

.00 
.00 

.on 

.14 
.11 
.12 
.12 

222-286 

1              

.12 

.11 

.11 
.09 
.07 

.072 
.OH 

.088 

.009 

.006 

.002 
.002 

.(MM) 

.098 

.073 

.072 
.068 
.087 

220-230 

6 

.17 

.17 
.It, 
.11 
.10 

4.12 

3.73 
3.71 
3.(13 
2.  63 

12.80 

12.80 
L2.77 
12.64 

220  230 

r,  

9.16 
'.i.  L2 
H.(i7 

220-280 

7  

216-226 

.266 

4 

B 

.16 

B 

.III.", 

8 

t 

! 

.  124 

3 

4.84 
1 
B 

...:m 

12.  S3 
4 

t 

9.21 
B 
4 

.14 

2 
I 

221-231 

3 

8 



- 

ANALYSES    OF    CERTIFIED   PERMITTED    COLORS.  199 

Orange  I. 

[  Figures  calculated  to  100  parts  pure  color,  and  arranged  in  the  order  of  their  size.  Figures  in  the  same 
horizontal  line  do  not  refer  to  the  same  sample;  the  dash  line  shows  the  location  of  the  average  of  each 
column.] 


Number  of 
batches. 

Insoluble. 

Ether  extractives. 

Com- 
mon 
salt. 

So- 
dium 

sul- 
phate. 

Sul- 
phur. 

So- 
dium. 

Cal- 
cium. 

Total. 

Inor- 
ganic. 

Neu- 
tral. 

Alkali. 

Add. 

Total. 

1 

0.39 

.38 
.28 

.23 

.23 

0.18 

.08 
.08 

0.224 

.220 
.210 

.207 

.181 

.177 
.174 

0.093 

.060 
.043 

.035 

.035 

0.08 

.077 
.067 

.055 

0.360 

.309 
.306 

.300 

,2 

.267 

3.13 

3.13 
3.04 

2.36 

0.22 

9.26 

9.23 
9.12 

9.10 

9.06 

9.06 

9.05 

9.02 

6.82 
6.76 

6. 62 

0.29 

2 

.10 

.24 

3 

.24 

4 

05 

.04 

.04 

.03 

.03 

.02 


5 

.048 
.039 
.036 

.029 
.010 

1.9S 

1.91 

1.90 

1.41 

1.05 
1.01 

6.54 
6.48 
6.32 
6. 21 

.05 

6 

.16 
.15 

.11 

.10 
.05 

.020 

.018 

.015 

.('11 
.011 

.04 

7 

.  246 

.2-24 

.175 
.124 

s       

.124 

.107 
.097 

9 

8.96 
8.  IS 

10 

Average 

Above 

Below 

.21 
6 
5 

.06 
3 

0 

.172 
7 
3 

.034 
5 
5 

.050 
1 
5 

.258 

6 
4 

2.09 
4 
6 

.03 
1 

1 

9.00 
8 
2 

6.55 
4 
4 

.18 

4 
2 

Amaranth. 

[Figures  calculated  to  100  parts  pure  color  and  arranged  in  the  order  of  their  size.  Figures  on  the  same 
horizontal  lines  do  not  refer  to  the  same  samples;  the  dash  line  shows  the  location  of  the  average  of  each 
column.] 


Insoluble. 

Ether  extractives 

Com- 
mon 
salt. 

Sul- 
phur. 

Sodi- 
um. 

Calci- 
um. 

Number  of  batches. 

Total. 

Inor- 
ganic. 

Neu- 
tral. 

Alkali. 

Acid. 

Total. 

1 

0.43 

.  30 

.  23 

.21 

0.33 
.  30 

.19 

.15 
.10 
.10 

0.090 
.088 
.069 

.017 

0.030 

.017 
.009 

.007 

.017 
.015 

.014 
.012 
.012 
.012 

.101 
.100 

.060 

4.  is 
4.  lti 

3.73 
3.08 

2.70 

16.04 
16.80 
15.63 

15.61 

15.59 

15.58 

15.57 

15.57 

15.54 
15.52 

14.22 
14.19 
12.  10 

o  20 

2 

a 

17 

4 

11.47 
11.43 
11.43 
11.42 

11.38 

11.33 

11.32 
11.81 

1 1  28 

11.27 

11.27 

11.21 
11.  is 
11.1.-, 
11    14 

11.10 
11   Ol 

.14 

r, 

.  056 

.053 

.052 

.051 
.048 

.012 
.012 

.010 

.039 

.0.-. 

14 

r, 

.13 

.12 

.12 
.12 

.11 
.11 
.11 
.  11 

• 
.070 
.07 

.035 
.034 

.034 

.034 

.027 
.026 

.021 

.012 

.005 
.005 

.005 

.(Mi:, 

.mil 

.(HM1 

13 

: 

.06 
.06 

.04 

.04 

.03 
.08 

.02 

.02 

13 

.010 

.007 

.005 

.003 

12 



12 

10 

2.  62 

2.21 
2.  12 

2.  12 

1.U4 

1.91 
L01 

12 

n 

11 



14 

15.41 
15.41 
15.41 

IV  lo 
15.  12 

.07 
.00 

15 

16 

17 





20.      

21 

.148 

11 

.006 

7 
12 

4 

r, 

11 

13 

B 

.012 
7 
11 



200 


COAL-TAR  COLORS  USED  TX  FOOD  PRODUCTS. 


Light  Green  SF  Yellowish. 

[Figures  calculated  to  100  parts  pure  color  and  arranged  in  the  order  of  their  size.  Figures  in  the  same 
horizontal  line  do  not  refer  to  the  same  sample;  the  dash  line  shows  the  location  of  the  average  of  each 
column.] 


Number  of 

batches. 

Insoluble. 

Ether  extractives. 

Com- 
mon 
salt. 

Sodi- 
um 
sul- 
phate. 

Sul- 
phur. 

Sodi- 
um. 

Calci- 
um. 

Total. 

Inor- 
ganic. 

Neu- 
tral. 

Alkali 

Acid. 

Total. 

1 

0.07 

0.034 
.02 

0.058 

0.011 

.007 

0.011 
.009 

0.076 

4.15 

0.00 

.00 

.00 
.00 
.00 

.00 

12.69 

12.27 

8.03 

7.99 

7.99 
7.94 
7.73 

4.52 

2 

.041 

.034 
.033 

.054 

.053 
.042 

.64 

.515 
.43 

.37 

.10 

3 

4 

.  03 
.02 
.02 

.01 

.01 
.01 
.01 

.01 

.00b 
.000 

.008 

.007 

12.07 
11.88 

11.88 

.09 
.06 
.OS 

1.56 



Aver   . 



Below 

.033 
2 

4 

.017 
2 
3 

.041 
3 

.006 

2 
2 

.008 
2 
2 

.  056 

1 
3 

1.221 

4 

.00 
0 
0 

12.16 
2 
S 

6.87 
5 

1 

.  96 

1 

Erythrosin. 

[Figures  calculated  to  100  parts  pure  color  and  arranged  in  the  order  of  their  size.     Figures  in  the  same  hoii- 
zontal  line  do  not  refer  to  the  same  sample;  the  dash  line  shows  the  location  o  the  average  of  each  column.] 


Insoluble. 

Ether  extractives. 

Com- 
mon 
salt. 

Sodi- 
um 
sul- 
phate. 

Sodi- 
um. 

Number  of  batches. 

Total. 

Inor- 
ganic. 

Neu- 
tral. 

Alkali. 

Acid. 

Total. 

Iodin. 

1   

0.13 
.09 

0.09 
.04 

0.039 
.039 

.  037 

0.017 
.009 

.oos 

0.051 

;       .048 

047 

1.13 
1.00 

.48 

0.00 
.00 

.00 

.00 
.00 
.00 

.00 
.00 
.00 

5.42 
5.35 

5.33 

5.29 
5.15 
5.11 

2         

3           

.  059 

.05 

.04 
.04 

.04 
.03 

.024 

.01 
.01 
.01 

.01 

56.  40 

4              

.034 
.033 
.033 

.027 

.  002 
.002 
.000 

037 

.23 

.09 
.09 

.09 
.09 
.036 

56. 07 

035 

035 

55.98 

6 

55.97 

7              

.027 

3.85 

55.94 

55.90 

g 



.059 
2 
6 

.028 
2 
5 

.  035 
3 
4 

.  006 

3 

3 

040 

3 

4 

.  360 
3 

6 

.00 

5.07 
6 
1 

56.  23 

3 

6 

1 

Indigo  disulpho  acid. 

[Figures  calculated  to  loo  parts  pure  color  and  arranged  in  the  order  of  their  size.  Figures  on  the  same  hori- 
zontal lines  do  not  refer  to  the  sumo  samples;  the  dash  line  shows  the  location  of  the  average  of  each 
column.] 


Number  <>f 

lies. 

Luble. 

Ether  i 

Com- 
mon 

salt. 

Bodi- 

um- 

sul- 
phate. 

Sul- 
phur. 

Sodi- 
um. 

Calci- 
um. 

Total. 

Inor- 
ganic. 

Neu- 
tral. 

Alkali. 

Acid. 

'total. 

1  .  .  .     . 

o.  50 

.  It, 

0.28 

.21 

O.  1  10 

.Old 

0.320 

.217 

6.77 

16.  12 

10.22 

18.  15 

18,  12 

lo.  18 
9.90 
9.64 

0.  45 

.026 

.021 
.00, 

.13 

:<        

.  102 

.088 

.07.", 

.015 

.018 

.113 

.  1  II 

4.79 

.110 

.00 
.00 

.43 
.  32 

2. 89 
1.85 

.  to 

.  i ).', 

.  22 

.  16 

13.  I.", 

9.  13 

Y  5 1 

i, 

A\ci 

Bekw  . 

:< 

.  235 

1 

2 
3 

2 

8 

.011 

i 

.189 

•> 
8 

3.  1  2 

3 

1 

I 

9.49 

1 
2 

.  L9 

1 
3 

ANALYSES    OF    CERTIFIED    PERMITTED    COLORS. 


201 


COMPARISON  WITH  ANALYSES  MADE  LN  1907. 

A  comparison,  as  far  as  possible,  of  these  figures  with  the  corre- 
sponding data  previously  given  for  samples  on  the  market  in  the 
summer  of  1907  is  made  in  the  following  table.  The  figures  in  this 
new  table  show  the  value  of  the  fraction  obtained  by  dividing  the 
old  average  figure  by  its  corresponding  new  average  figure — that  is, 
they  show  how  many  times  greater  the  old  average  figures  are  than 
the  corresponding  new  average  figures.  Italics  indicate  those  items 
in  which  there  has  been  a  retrogression  hi  the  new  figures  as  com- 
pared with  the  old;  all  the  other  figures  represent  an  advance.  It 
will  be  noted  that  comparisons  are  not  made  for  Ponceau  3R  and 
Erythrosin.  Tins  comparison  was  omitted  because  there  was  but 
one  sample  of  Ponceau  3R  examined  and  a  partial  analysis  of  one 
sample  of  Erythrosin  in  the  old  work. 

Ratio  of  average  figures  of  1907  to  those  for  the  certified  colors,  1909. 


Salt. 

Insoluble. 

Ether  extr  u 

Color. 

Total. 

Vola.ile.      *E* 

Nonacid.      Acid. 

Total. 

Naphthol  Yellow  S 

4.88 
3.54 
15.07 
.66 
8.05 

4.44 
9.07 
11.26 

31.00 
3.29 

9.02             0.67 

7.50           °l-89 

15.97 

Orange 

20.00 
21.40 

29.00 
5.4 

3.00 

7.71 

17.00 

1 .  57 
4.07 

.16 

10.77 

5.00 

Green 

Blue 

These  retrogressions  are: 

1.  Salt  in  the  Green. 

2.  Nonvolatile  insolubles  in  the  Yellow. 

3.  Nonacid  ether  extract  in  the  Green. 

4.  Nonacid  ether  extract  in  the  Blue. 

5.  Total  ether  extract  in  the  Blue. 

With  respect  to  the  first  of  these  retrogressions  there  is  this  to  be 
said:  One  lot  of  Green  had  apparently  been  purified  by  precipitation 
with  salt,  since  it  was  in  every  other  respect  of  a  high  quality  that 
is,  it  was  free  from  arsenic  and  heavy  metals  within  the  pharmacop 

and  its  ether  extractives  were  very  satisfactory.     The  other  lots 
rreen  examined  had  apparently  not  been  made  in  this  manner. 

With  respect  to  the  second  retrogression,  the  probable  explanation 
is  that  some  of  the  lots  were  made  during  a  period  when  the  municipal 
water  supply  was  excessively  hard,  as  before  explained.  The  remain- 
ing three  retrogressions  are  probably  due  to  the  fact  that  the 
methods  of  analysis  used  were  not  so  accurate  as  the  methods  later 
employed  and  hereinafter  described  (pp.  223 

It  will  be  noted  that  in  three  of  the  six  batches  of  Indigo  disulpho 
acid  reported  there  is  no  sodium  Bulphate;  whereas  in  the  other  three 
lies  the  amount  of  this  substance  is  as  high  as  16.12.     The 

for  this  LS  that    in   the  early  Btages  Of  the  work   the  results  obtained 


202 


COAL-TAK  COLORS  USED  IN  FOOD  PRODUCTS. 


by  the  manufacturers  pointed  in  the  direction  of  the  impossibility  of 
getting  rid  of  all  the  sodium  sulphate;  but  later  and  more  extended 
work  showed  tins  conclusion  to  be  an  error.  There  is  therefore  no 
good  reason  for  permitting  sodium  sulphate  as  a  contaminant  in  this 
or  any  other  of  the  seven  products. 

CONFORMITY    OF  ANALYTICAL    DATA    WITH    THEORETICAL    COM- 
POSITION. 

The  seven  tables  following,  likewise  based  upon  the  74  Govern- 
ment analyses,  show  the  conformity  or  nonconformity,  as  the  case 
may  be,  of  these  samples  with  their  theoretical  composition.  The 
second  and  third  columns  show  the  percentage  based  on  theory  of 
the  contained  sulphur  and  sodium  in  the  case  of  all  colors  except 
Erythrosin,  where  the  figures  for  iodin  are  substituted  for  those  of 
sulphur.  The  fourth  column  shows  the  actual  ratio  of  sodium  to  sul- 
phur or  iodin,  as  the  case  may  be,  and  the  fifth  column  gives  the 
percentage  of  the  figure  of  column  4  based  on  the  theoretical  value 
winch  is  given  in  parentheses  at  the  head  of  colunms  4  and  5.  The 
summary  gives  the  maximum,  minimum,  and  average  of  each  column. 
Taken  as  a  whole  the  figures  are  fairly  satisfactory  and  show  a  rea- 
sonable conformity  of  the  actual  product  to  theoretical  requirements, 
although  there  seems  to  be  considerable  room  for  improvement,  which 
no  doubt  can  be  achieved  in  time. 

1'iircntages  based  on  theoretical  composition. 
NAPHTHOL  YELLOW  B. 


Number 
of 

Sulphur. 

Sodium. 

Na 

s  =(1.4379). 

Number 
of 

batches. 

Sulphur. 

Sodium. 

Na 

-g  =(1.4379). 

batches. 

Value. 

Per  cent. 

Value. 

Percent. 

l 

Per  cent. 
103.  120 
90.312 
97.  205 

Per  cent. 
103.  10 

9'.).  068 

100.  (MM) 

1.4:577 
1.4791 
1.4792 
1.4707 

99.983 
102.860 

102.870 

102.  270 

10 

11 

12 

13 

Per  cent. 
98.880 
98.658 

KM).  330 
100. 100 

Per  a  ui. 
101.06 
101.22 

100.15 
100.00 

1.4578 
1.4631 
1.  1353 

101.36 

2 

101.74 

3 

4 

97.  642 

'W.VKI 

.-, 

Average. . 



Min 

0 

99. 101 
103.120 

90.312 

102.212 

1 03.  .->00 

1.4.j7S 
l.  L792 

101. S7S 

7 

98.  992 
99.331 

1(H).  HI) 

8 

100.15 
103.50 

1.4498 

100.  SO 
102.  IS 

99.82G 

9 

PONCE 


N 

urilxT 
of 

Sulphur. 

Sodium. 

0.719..:,). 

Number 

of 

Sulphur. 

Sodium. 

Value. 

Per  cent. 

Value. 

Percent 

1 

Pert  i  nt. 

J'i  r  a  nl. 
93.617 

9a  i7i 

8 

9 

Avenge. 
lias 

.Mm  ... 

l'ir  cent. 

Per  ct  ui. 
101.920 
L01.700 

0.74296 

103.33 

102.48 

100.  110 

.70518 
.71892 

98.662 
99.918 

lol.  16 

4 

99. 266 

11MI.   10 

97.  AM 

98.  73S 
101.920 
98.617 

.Tints 

99. 144 

1 

f. 

ANALYSES    OF   CERTIFIED    PERMITTED    COLORS. 


203 


Percentages  based  on  theoretical  composition — Continued. 
ORANGE   I. 


Number 
of 

Sulphur. 

Sodium. 

Na 
s  =(0.71905). 

Number 

of 
batches. 

Sulphur. 

Sodium. 

Na 

.71905). 

batches. 

Value. 

Per  cent. 

Value. 

Percent. 

1 

2 

z. '.'.'.'... '. 

4 

s 

88.972 
100.76 
101.09 
99. 135 
99. 135 
97.810 
98.799 

100.44 
103. 72 
102.53 

0. 81226 
.73002 

112.97 
102. 77 
101.53 

8 

9 

10 

Average . 

Max 

Min 

98. 471 
99.563 
99.342 

85.901 
99. 241 
98. 330 

0.70066 
.71710 
.71208 

97.454 
99.740 
99.042 

98.308 
101.09 
88.972 

99.376 
103. 72 
95.901 

.72957 
.81226 
.69309 

101.475 

o 

7 

94.  234 
100.610 

.69309 
. 73243 

96. 391 
101.90 

112.97 

AMARANTH. 


, 

96. 795 

105.  76 

0.  78519 

2 

98. 176 

99. 037 

.72488 

3 

94. 975 

124.29 

.94048 

4 

94. 975 

124.04 

. 93849 

o 

100.750 

96.240 

.68637 

b 

99.246 

99.911 

. 72341 

7 

97. 174 

100.260 

. 72454 

8 

96.929 

99. 827 

.74011 

9 

97. 926 

97.  465 

.71820 

10 

96. 975 

97. 990 

. 72744 

11 

96.  733 

97. 389 

.72338 

12 

97.  487 

98.514 

.72615 

13 

96.798 

97. 028 

. 72030 

109.21 
100.82 
130.80 
130.53 

95. 470 
100.62 
100.78 
102.94 

99. 476 
101.18 
100.62 
100.99 
100.18 


Average . 
Max 

Min 


97.800 
97.  499 
97. 614 
97.499 
97.863 
98. 052 
97.800 
97. 735 


97.467 
100.750 
94. 975 


98.  863 
99.911 
98.950 
99.476 
98.689 
98.  393 
98.514 


0.  72640 
.73646 

.73325 
.  72465 
.72106 


101.347 
124.  29 
96.240 


. 74707 
. 9404S 


loi.  as 

102.  43 
101.32 
101.98 
loo. 78 
100.05 
100.  68 
99.914 


103.90 
130.80 
95.  470 


LIGHT   GREEN   BF  YELLOWISH. 


1 

102.85 

6 

104.50 

95.  547 

0.65783 

2 

98.148 

93.018 
98. 020 
96.148 

3 

4 

5 

109.87 
106.23 
102.35 

0.60911 
.65358 

90.911 
93.  540 

•  Average. 
{  Min 

105.  26 
109.87 

95.  498 

96.029 
93.018 

.6482/ 
?67256 
.60911 

90.167 

ERYTHROSIN. 

Number 
of 

Iodin. 

Sodium. 

1  2 

Number 

of 
batches. 

Iodin. 

Sodium. 

090855). 

batches. 

Valt  if. 

Per  cent. 

1 

2 

a 

4 

5 

Per  cent. 
98.915 
97.061 

97.780 

97.209 

97.035 

Per  cent. 
ft.  473 

98.  277 

1 
.000604 

75.  so;, 
104.00 

1. 

9 

\ \« rage. 

Min 

96.  879 

102.09 

.005741 

97. 952 

73.  178 

.090204 

99.146 

<; 

101.71 

204 


COAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 

Percentages  based  on  theoretical  composition — Continued. 
INDIGO  DISULPHO  ACID. 


Number 
of 

Sulphur. 

Sodium. 

^:1  =  (0.71905). 

Number 
of 

Sulphur. 

Sodium. 

N*a=  (0.71905). 
S 

batches. 

Value. 

Per  cent. 

batches. 

Value. 

Percei  t. 

1 

2 

3 

4 

5 

Per  cent. 
97. 670 
95.636 
97.600 
96. 148 
97. 382 

Per  cent. 
103.  330 

98.279 
103. 760 

91.926 
106.560 

0. 71482 
.69430 
.71832 
.64598 
. 73934 

99.423 
95.669 
99.910 
89.848 
102. 830 

6 

Average . 

Max 

Min 

Per  cent. 
97. 818 

Per  cent. 
109.040 

. 75315 

104. 750 

97.042 
97. 818 
95.630 

102. 149 
109. 040 
91.926 

.71099 
.75315 
.64598 

98.738 
104. 750 
89.848 

ARSENIC  DETERMINATIONS  ON  86  BATCHES. 

During  the  course  of  tliis  work  it  became  necessary  to  determine 
the  exact  amount  of  arsenic  contained  in  86  of  the  various  batches 
of  certified  colors;  for  this  purpose  the  arsenic  method  of  Seeker  and 
Smith  (see  p.  212)  was  devised.  These  results  are  expressed  in  the 
number  of  parts  of  color  containing  one  part  of  metallic  arsenic  (As). 
The  numbers  in  parentheses  indicate  the  number  of  specimens  of  the 
quality  indicated. 

Xaphthol  Yellow  S  (17  specimens).— 770,000,  833,000,  1,250,000  (2),  1,428,000  (2), 
1,666,000  (3),  2,000,000  (6),  3,333,000  (2). 

Ponceau  (15  specimens).— 588,000,  625,000,  667,000,  714,000  (2),  769,000  (2), 
1,000,000  (2),  1,111,000,  1,250,000,  1,666,000  (2),  2,000,000,  2,500,000. 

Orange  (7  specimens).— 200,000,  250,000,  588,000,  1,000,000,  1,111,000,  1,429,000, 
5,000,000. 

Amaranth  (27  specimens).— 909,000, 1,000,000,  1,111,000,  1,250,000  (2),  1,438,000  (3), 
2,000,000(4),  2,500,000  (4),  3,333,000  (9),  5,000,000  (2). 

Green  (8  specimens). —166,000,  200,000,  370,000  (2),  500,000,  666,000,  770,000,  833,000. 

Eryihrosia  (7  specimens).— 2,000,000(2),  5,000,000  (2),  10,000,000  (2),  20,000,000  (1). 

Blue  (5  specimens).— 285,000,  666,000,  1,428,000,  3,333,000  (2). 

The  United  States  Pharmacopoeia  test  for  arsenic  is  sensitive  to 
0.005  mg  of  arsenious  oxid  (As203)  which  on  a  sample  containing  2 
grams  of  actual  or  real  color  would  amount  to  one  pari  of  arsenious 
oxid  in  400,000  of  color;  calculated  to  metallic  arsenic,  the  basis 
employed  in  the  foregoing,  this  would  mean  528,000  parts  of  color  for 
each  one  part  of  metallic  arsenic. 

There  are,  therefore,  in  the  foregoing  86  lots  of  certified  colors 
hich  did  not  comply  with  thai  requirement,  namely: 

Orange  (2  specimens).— 200,000  and  250,000. 

Green    (5  specimens).— 166,000;  200,000;  370,000   (2);  500,000. 

Blue  (l  specimen). — 285,000. 

The  reason  for  this  discrepancy  is  thai  in  the  preparation  of  the 
samples  for  analysis  by  the  United  Stales  Pharmacopoeia  test  a  loss 
of  arsenic  ensued,  which  is  avoided  in  the  Seeker-Smith  method 
now  employed  in  making  these  determinations.     Had  the  existence 


ANALYSES    OF    CERTIFIED    PERMITTED    COLORS.  205 

of  this  discrepancy  been  proven  at  the  time  the  first  analysis  was 
made  certification  would  have  been  denied  to  the  eight  lots  above 
mentioned. 

These  results  further  show  the  position  taken  early  in  the  work 
by  several  of  the  manufacturers — that  a  requirement  of  not  more 
than  1  part  of  metallic  arsenic  in  not  less  than  264,000  parts  of 
coal-tar  color  could  not  be  complied  with  on  a  commercial  scale 
to  be  untenable;  on  tins  basis  only  4  out  of  the  86  lots  examined 
would  have  been  excluded.  Further,  the  position  of  some  manu- 
facturers and  dealers  that  the  arsenic  requirement  ought,  for  prac- 
tical manufacturing  reasons,  not  to  be  more  rigorous  than  one  part 
of  metallic  arsenic  in  26,400  parts  of  color,  or  1  part  of  arsenious 
oxid  (As203)  per  20,000  parts  of  color,  is  not  borne  out  by  the  data. 

SUGGESTED   REQUIREMENTS    FOR   CERTIFIED    COLORS. 

Although  the  material  embodied  in  this  report  gives  a  very  good 
idea  of  the  composition  and  quality  of  substantially  30  different 
lots  of  permitted  colors  prior  to  the  issuance  of  Food  Inspection 
Decisions  Nos.  76  and  77,  and  of  74  lots  of  certified  colors,  yet  these 
data  are  hardly  sufficient  to  furnish  a  basis  for  standards  with  winch 
each  color  specimen  must  comply  in  detail.  The  fitness  or  unsuit- 
ability  of  any  lot  has  been  determined  by  the  examination  of  the 
analytical  data  obtained  thereon  in  the  Food  and  Drug  Inspection 
Laboratory  at  New  York;  such  examination  has  been  applied  to 
the  particular  color  under  investigation  with  respect  to  its  general 
relationship  to  the  results  theretofore  achieved.  If  in  some  minor 
quality,  as,  for  example,  freedom  from  salt,  the  sample  was  not  up  to 
what  had  been  previously  accomplished,  but  in  a  major  quality,  as 
for  example,  ether  extractive,  it  was  equal  to  or  better  than  what 
had  been  previously  accomplished,  and  the  pharmacopoeia]  tests  for 
arsenic  and  heavy  metals  were  satisfied  with  the  exception  of  iron, 
and  the  amount  of  iron  was  within  die  limit  previously  stated, 
0.005  per  cent,  and  the  other  factors  showed  a  fairly  close  conformity, 
such  a  defect  as  its  salt  content  would  not  act  as  a  bar  to  the  pass- 
ing of  the  lot;  however,  no  matter  how  good  a  color  might  be  in 
respect  to  such  determinations  a-  ether  extractive,  if  it  failed  to 
comply  with  the  United  States  Pharmacopoeia  requirement  for 
arsenic  or  for  heavy  metals  it  was  not  accepted. 

These  arsenic  results  have  been  tabulated  to  show  the  distribution 
of  arsenic  content  (As,Ot)j  the  numbers  at  the  top  are  the  Green 

Table  numbers;   the  numbers  in   the  body  of  the   table  indicate  the 

number  of  specimens  of  the  arsenic  content  sti  ted  in  the  first  column ; 

the  last  column  shows  ihe  totals  of  all  colors  of  the  arsenic  content 

(As_(),,)  corresponding  thereto. 


206 


COAL-TAE    COLORS   USED   IK    FOOD   PRODUCTS. 
Arsenic  content  of  S6  lots  of  certified  colors. 


Arsenic 
content. 

Green  Table  numbers. 

Total. 

4 

56 

85 

107 

436 

517 

692 

1  part  in— 
1  126,200 

i  151.000 

1151,500 

i  189, 300 

1215,900 

i  280, 300 

i  378, 700 

44.").  400 

473,500 

504,600 

505, 300 

540, 900 

582, 500 

583,300 

631,000 

688, 700 

757,500 

841,600 

946,900 

1,081,000 

1,082,000 

1,089,000 

1.262.000 

1,515.000 

1,893,000 

2,524.000 

3,787,000 

7.157,000 

15, 150, 000 

il 
il 

1 

1 
1 
1 
1 
2 

1 

2 

1 

1 
2 
2 
2 
2 
1 
4 
3 
5 
3 

3 
5 

13 

5 
13 

5 
2 

1 

1  1 

il 

l  2 
i  1 

1 

1 

1 

1 

1 

...... 

1 
2 
2 

1 

1 

1 
1 

1 
2 

2 

2 
1 
1 

1 
1 

1 

1 

3 

3 
6 

2 

1 

4 
4 
9 
2 

2 

2 

1 

2 
2 

1 

17 

15 

7 

27 

8 

7 

5 

86 

i  The  certification  of  these  lots  was  due  to  an  unknown  source  of  error  in  the  analytical  method;  the 
analyses  made  at  that  time  (July,  1909),  showed  less  than  1  part  of  AS2O3  per  400,000;  see  also  page  204. 

It  is  therefore  somewhat  premature  to  attempt  to  define  rigidly 
the  requirements  for  composition  and  purity  for  colors  until  a  suffi- 
cient number  of  analyses  is  available  to  permit  a  hard-and-fast  line 
to  be  drawn  for  each  item  as  required  for  each  color.  Until  that 
time  the  decision  as  to  whether  or  not  a  certain  color  shall  be  cer- 
tified must  rest  with  the  Department  of  Agriculture.  However, 
the  following  requirements  are  tentatively  suggested  as  being  com- 
mercially  practicable.  It  should  be  clearly  understood  that  the  ten- 
tative requirements  here  stated  are  based  on  the  results  of  actual 
control,  and  are  not  any  more  searching  or  numerous  than  arc  the 
requirements  for  many  if  not  most  of  the  coal-tar  dyes  or  their  com- 
ponent parts  in  the  industrial  arts,  particularly  for  the  various  kinds 
of  paint,  varnish,  and  ink  making.  While  it  may  be  that  some  of  the 
tentative  requirements  herein  defined  necessitate  the  expenditure  of 
considerable  work  and  time,  yet  that  is  also  true  of  some  of  the 
commercial  requirements,  since  manufacturers  of  cheap  paints, 
varnishes,  inks,  and  the  like,  find  it  wise  and  necessary  carefully  to 
control  i\w  quality  of  the  coal-tar  dyes  or  their  component  parts 
which  they  use,  it  can  not  be  less  wise  or  accessary  to  extend  the 
same  kind  of  quality  control  to  those  coal-tar  dyes  intended  and  sold 


ANALYSES   OF    CERTIFIED    PERMITTED    COLORS. 


207 


for  human  consumption  as  food.  This  stand  is  fully  justified  by  the 
quality  of  the  coal-tar  dyes  offered  as  food  colors  on  the  United  States 
markets  as  described  in  the  foregoing  pages.  That  such  control  is 
not  only  practical,  but  practicable,  is  fully  proved  by  the  fact  that 
more  than  20.5  tons  (41,000  pounds)  of  coal-tar  food  dyes  have  been 
so  controlled,  examined,  and  certified  under  the  food  inspection  deci- 
sions hereinbefore  mentioned. 

The  figures  are  expressed  in  parts  per  hundred  of  actual  color 
contained  in  the  dye  and  not  in  parts  per  hundred  of  the  total 
substance.  The  numbers  at  the  head  of  the  columns  are  the  num- 
bers in  the  Green  Tables. 


Tentative  limits  of  composition  suggested  for  permitted  colon. 

(Parts  per  hundred  of  actual  color.; 


Determinations. 


Insolubles: 

Total 0. 070 


Nonvolatile  on  ignition 
Ether  extractives: 

Neutral 

Alkaline 

Acid 

Common  salt 


Green  Tables  numbers. 


■ 

107 

43.5 

- 

692 

0.070 

0.270 

0.250 

0.  130 

0.030 

0.000 

0.  4.50 

.040 

.150 

.  050 

.050 

.010 

.020 

.250 

.017 

.090 

.  150 

.030 

.040 

.035 

.100 

.004 

.015 

.03.5 

.  00.5 

.006 

.002 

.030 

.060 

.017 

.050 

.010 

.008 

.  150 

.000 

5.000 

2.000 

2.500 

.600 

.400 

3.000 

In  addition  to  these  there  are  the  following  requirements  applicable 
to  all  colon  : 

1.  The  absence  of  admixed  dye  must  be  convincingly  demonstrated  by  suitable 
test. 

2.  Arsenic. — Test  17  of  the  United  States  Pharmacopoeia,  1900,  applied  to  so  much 
of  the  specimen  as  represents  3.5  grama  of  actual  dye  must  give  a  negative  response. 
Such  negative  result  must  be  reenforeed  by  a  check  test  identical  with  the  test  on  the 
dye  with  the  addition  of  0.005  mg  of  arsenic  (\s,03)  to  the  dye  prior  to  treatment, 
and  this  check  test  must  produce  a  positive  result  for  the  presence  of  arsenic.  Igni- 
tions in  the  preparation  of  ihe  material  for  the  test  must  be  made  in  porcelain. 

Any  other  mode  of  testing  which  is  demonstrated  to  be  capable  of  detecting  0.005 
in.-.!  Ided  arsenic  (AftjOj)  in  so  much  of  the  specimen  as  represents  3.5  grams  of  actual 
color  will,  of  course,  1"'  accepted.  This  quantity,  however,  is  only  tolerated  tenta- 
tively pending  further  investigations  relative  to  the  complete,  or  practically  com- 
plete, elimination  of  arsenic  from  foods,  especially  those  which  are  largely  used  by 

children,  such  as  candies. 

."..  linn  ij  in,  tuis.    Test  l-i  of  the  United  States  Pharmacopoeia  as  revised  May  l, 
L90T,  using  so  much  of  the  specimen  as  represents  one  part  of  actual  dye  must 
negative  response  for  all  metals  except  iron,  which  may  be  present  in  amounts 

I  of  0.006  per  cent  of  iron  based  on  t  he  d\  e  actually  present  in  the  specimen. 

4.   None  of  the  d;  1   for  certification  shall   contain  any  dauber's  salt   or 

sodium  sulphate  in  any  farm,   nor  shall  they  contain  any  added  BUgar,  dextrin,  or 
other  loader,  tiller,  or  reducer  for  any  purpose  whatsoever,  and  Convincing  proof  Of  the 
.  any  or  all  of  them  must  DO  Submit 


208         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

5.  The  ether  extractives  are  to  be  made  successively  upon  water  solutions  of  the 
dye,  first  neutral,  then  made  alkaline  with  caustic  soda,  and  then  made  acid  with 
hydrochloric  acid,  using  washed  or  sodium,  dried  ether. 

6.  The  sulphur  content  of  the  sulphur-containing  dyes  must  agree  substantially 
with  the  theoretical:  likewise  the  sulphated  ash  figures  of  all  must  agree  substantially 
with  the  theoretical;  variations  between  these  two  sets  of  figures,  as  long  as  they  are 

stent  with  each  other,  will  not  be  reason  for  rejection. 

7.  In  the  case  of  No.  4  proof  must  be  submitted  showing  that  the  specimen  is  of  the 
sodium  or  potassium  variety,  and  if  it  is  a  mixture  of  these  two  varieties  the  proportion 
of  each  present  in  the  mixture  must  be  stated. 

8.  In  the  case  of  Xo.  5G  the  crude  cumidin  employed  may  have  a  boiling  point  of 
from  220°  to  230°  C,  and  may  be  liquid  or  solid;  the  absence  of  any  compound  of 
S  or  G  salt  must  be  convincingly  shown. 

9.  In  the  case  of  No.  85  convincing  proof  must  be  submitted  that  beta-naphthol 
orange  if  present  at  all  is  present  in  an  amount  not  in  excess  of  5  per  cent  of  the  coal- 
tar  dye  present. 

10.  In  the  case  of  Xo.  107  the  absence  of  any  compound  of  S  or  G  salt  must  be 
convincingly  shown. 

11.  In  the  case  of  Xo.  435  the  product  should  be  free  from  calcium ;  convincing  proof 
of  absence  of  Xo.  434  must  be  submitted. 

12.  In  the  case  of  Xo.  517  the  actual  dye  must  contain  not  less  than  56  per  cent  of 
iodin  (sodium  basis)  and  must  not  contain  any  other  halogen;  the  kind  and  amount 
of  metallic  base,  whether  sodium,  potassium,  or  the  like,  must  be  shown. 

13.  In  the  case  of  No.  002  the  absence  of  indigo  monosulphonic  acid  and  of  nonsul- 
phonated  indigo  must  be  convincingly  shown. 

14.  Each  foundation  certificate  must  be  tiled  in  duplicate,  but  need  not  be  executed 
in  duplicate  and  must  contain  a  summarized  or  tabulated  statement  of  all  the  quan- 
titive  results  contained  in  the  certificate,  also  a  tabulation  or  summary  of  the  quali- 
tative tests  made,  together  with  the  results  of  such  tests,  all  stated  on  one  sheet,  so 
that  the  certificate  will  bear  within  itself  its  own  summary  and  conclusions. 

15.  The  fundamental  analytical  data  must  be  given  with  such  fullness  as  to  permit 
efficient  checking  of  the  calculations,  and  the  arithmetical  operations  performed 
should  be  indicated  wherever  needful  to  avoid  confusion,  or  to  facilitate  the  work  of 
the  checking  chemist,  or  make  the  meaning  of  the  certificate  more  plain. 

There  are  freely  quoted  in  the  United  States  market  two  substances, 
paranitranilin  and  betanaphthol,  which  are  subject  to  much  com- 
petition, the  prices  for  which,  wholesale,  are  not  far  from  25  cents 
and  9  cents,  respectively.  A  specimen  of  each  lias  been  examined, 
and,  as  before  stated,  they  have  both  been  found  to  be  of  such 
purity,  with  respect  to  arsenic,  heavy  metals,  and  general  cleanliness. 
that  had  they  been  capable  of  use  in  food  products,  no  objection 
against  their  use  on  this  score  could  reasonably  be  raised;  certainly 
no  such  objection  could  be  successfully  maintained. 

The  following  table  discloses  the  chemicals  entering  into  the  manu- 
facture of  paranitranilin  and  of  betanaphthol,  as  well  as  of  each 
of  the  seven  permitted  colors;  the  ingredients  numbered  1  to  7  are 
used  in  the  manufacture  of  these  two  substances,  as  well  as  in  the 
seven  permitted  colors,  as  indicated  by  the  "x"  entries;  ingredients 
8  to  20  are  used  only  in  the  manufacture  of  the  seven  permitted 
colors,  and  not  in  paranitranilin  and  betanaphthol. 


ANALYSES   OF    CERTIFIED   PERMITTED   COLORS. 


209 


Comparison  of  chemicals  entering  into  the  composition  of  the  seven  permitted  colors  and 
of  paranitranilin  and  betanaphthol. 


Determinations. 

4. 

Xap- 

thol 

Yellow 

S. 

56. 

Pon- 
ceau 
3R. 

85. 
Orange 

107. 

Ama- 
ranth. 

435. 

Light 
Green. 

517. 

Ery- 
thro- 
sin. 

692. 
Indigo 
disul- 

pho 
acid. 

Parani- 
trani- 
line. 

■&    Q.  O 

X 

X 

X 
X 
X 

X 

X 
X 

X 
X 

X 
X 
X 
X 
X 

X 

X 

X 
X 
X 
X 

X 
X 
X 

X 
X 

X 

X 
X 

X 
X 
X 

X 
X 

X 

I 

X 

2.  Benzol 

3.  Sulphuric  acid '       x 

X 

5.  Metallic  iron ' 

6.  Acetic  acid 

X 

X 
X 

7.  Caustic  soda  or  potash ...       x 

X 

Carbonate  of  soda 

Common  salt 

Wood  or  methyl  alcohol. 

Lime 

Hydrochloric  acid 

Sodium  nitrite 

Ethyl  chlorid 

Peroxid    of   lead    or    of 

manganese 

Phosgene 

Iodin 

Metallic  mercury 

Ferric  chlorid 

Chlorin 


11 


Id 


Id 


With  respect  to  the  arsenic  content  of  the  finished  product,  it  can 
be  asserted,  without  any  fear  whatever  of  successful  contradiction, 
that  the  arsenic  finds  its  way  into  the  goods  by  way  of  the  sulphuric 
acid  which  is  used  in  the  manufacture  of  all  the  permitted  colors,  as 
well  as  in  the  manufacture  of  Paranitranilin  and  Betanaphthol.  If 
arsenic  from  this  source  can  be  kept  out  of  these  substances  it  can 
also  be  excluded  from  the  permitted  colors. 

Turning  now  to  those  ingredients  below  the  parallel  lines,  the  only 
means  of  introducing  arsenic  would  be  through  the  hydrochloric  acid 
used,  which  in  turn  derives  its  arsenic  from  the  sulphuric  acid  used 
in  its  manufacture,  and  since  arsenic  free-sulphuric  acid  can  be  used 
in  the  first  stages  of  producing  the  seven  permitted  colors  and  tho 
paranitranilin  and  betanaphthol,  itcan  also  be  employed  in  the  manu- 
facture of  the  hydrochloric  acid  used  in  the  subsequent  stages  of 
manufacture  of  the  seven  permitted  colors.  Therefore,  it  seems 
unreasonable  to  permit  a  higher  arsenic  content  in  food  colors  than 
in  paranitranilin  and  betanaphthol,  which  are  sold  in  open  com- 
petition, and  which  are  used  for  the  production  of  tho  very  cheapest 
colored  cloths,  inks,  and  paints. 

With  reference  to  the  content  of  iron,  and  other  heavy  metals 
which  satisfied  the  pharmacopuial  tests  in  the  ease  of  paranitranilin 

and  betanaphthol,  these  materials  probably  enter  the  product  from 
tho  vessels  in  which  the  manufacturing  operations  are  performed. 

The  same  hind   of  vessel    used  in   the  manufacture  of    paranitranilin 
•1    -  -Bull.  147—12 14 


210        COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

and  betanaphthol  is  used  in  making  the  seven  permitted  colors,  and 
since  the  heavy  metals  can  be  and  are  kept  out  of  these  two  substances 
to  the  extent  required  by  the  Pharmacopoeia,  there  seems  to  be  no 
good  reason  why  they  should  not  be  kept  out  of  the  seven  permitted 
colors  when  made  for  use  in  food  products. 

Since  all  these  defects  in  the  seven  permitted  colors  can  be  obviated 
in  their  first  stage  of  manufacture  (as  is  shown  in  the  case  of  para- 
nitranilin  and  betanaphthol,  and  in  some  actual  commercial  samples 
of  1907,  see  sections  XIV  and  XV),  they  are  commercially  avoidable 
at  subsequent  stages  of  manufacture,  and  there  is  no  good  reason  why 
they  should  be  then  introduced. 

XVII.  METHODS  OF  ANALYSIS  USED  IN  TESTING  COLORS  FOR 

CERTIFICATION. 

INTRODUCTION. 

The  exact  analytical  methods  developed  and  tested  in  the  New 
York  Food  and  Drug  Inspection  Laboratory  and  used  in  obtaining 
the  analytical  data  contained  in  the  preceding  chapter  are  described 
in  the  following  pages.  These  descriptions  were  written  by  A.  F. 
Seeker,  of  that  laboratory,  under  whose  immediate  supervision  all  the 
laboratory  work  was  done,  and  they  represent  a  great  deal  of  work, 
extending  over  more  than  three  years.  The  methods  are  submitted 
in  the  hope  and  expectation  that  in  their  wider  application  by  a  larger 
number  of  chemists  any  defects  in  the  methods  or  conclusions  drawn 
from  the  results  will  be  detected  and  rectified.  Experience  in  the 
New  York  laboratory  has  shown  that  even  different  chemists  of 
varying  degrees  of  experience  in  this  particular  line  of  work  obtain 
concordant  duplicates  after  a  comparatively  short  laboratory 
acquaintance  with  these  methods. 

The  identity  of  these  colors  and  their  freedom  from  foreign  dyes  is 
shown  by  the  close  agreement  of  their  elements,  as  determined  by 
analysis,  with  their  theoretical  composition;  their  behavoir  toward 
reagents  as  given  by  standard  works  on  dyes;  their  distribution 
between  the  layers  when  neutral,  alkaline,  and  acid  aqueous  solutions 
are  shaken  with  various  immiscible  solvents;  uniformity  of  shade  in 
the  spots  produced  by  particles  of  the  dry  color  blown  over  the  surface 
of  wet  filter  paper,  or  water,  and  over  concentrated  sulphuric  acid; 
uniformity  of  shade  produced  by  a  0.5  per  cent  dyeing  on  wool  under 
standard  conditions,  with  similar  dyeings  from  fractions  produced  by 
partial  precipitation,  by  partial  salting  out,  by  fractional  crystalliza- 
tion, and  by  extraction  with  alcohol  or  some  liquid  in  which  the  pure 
color  is  not  very  soluble;  and  the  behavior  of  the  dye  in  acid  and 
alkaline  solution  toward  cotton.  Which  of  these  tests  are  Deeded  to 
prove  conclusively  the  identity  of  certain  dyes  or  to  establish  their 


METHODS  OF  ANALYSIS  FOE   CERTIFIED   COLORS.  211 

absence,  is  a  matter  that  varies  so  much  from  case  to  case  that  it  must 
be  left  largely  to  the  individual  judgment  to  decide  on  the  best  com- 
bination of  tests,  and  for  that  reason  such  combinations  are  not  here 
offered.  The  general  methods  and  procedures  just  outlined  have, 
however,  when  properly  combined,  led  to  satisfactory  results. 

In  order  to  compare  the  results  of  the  color  analyses  on  the  same 
basis,  the  actual  figures  obtained  in  the  various  determinations 
besides  being  reported  as  found,  are  also  recalculated  on  a  basis  of 
100  parts  of  actual  color,  i.  e.,  the  sum  of  the  percentages  of  material 
which  is  not  coloring  matter,  such  as  moisture,  total  insoluble  matter, 
sodium  chlorid,  sodium  sulphate,  and  ether  extractives  is  deducted 
from  100  and  the  percentages  of  the  various  constituents  found 
divided  by  the  difference,  the  quotient  being  then  multiplied  by  100. 
The  percentage  of  sodium  in  actual  dye  is  calculated  from  the  sul- 
phated  ash.  The  methods  of  analysis  of  the  seven  permitted  colors 
of  Food  Inspection  Decision  No.  76  are  given  in  the  following  order: 


1.  Naphthol  Yellow  S. 

2.  Ponceau  3R. 

3.  Orange  I. 

4.  Amaranth. 


5.  Light  Green  S  F  Yellowish. 

6.  Erythrosin. 

7.  Indigo  Disulphoacid. 


NAPHTHOL  YELLOW  S. 
MOISTURE. 


Dry  from  1  to  2  grams  of  the  finely  powdered  dye  in  an  air  oven  at 


120°  to  125°  C.  to  constant  weight. 

TOTAL   INSOLUBLE    MATTER. 

Dissolve  5  grams  of  color  in  200  cc  of  hot  distilled  water,  filter 
through  a  tared  gooch,  wash  till  the  washings  run  through  colorless, 
dry  the  insoluble  residue  at  105°  C,  and  weigh. 

NONVOLATILE    OR    INORGANIC    INSOLUBLE    MATTER. 

Ignite  the  gooch  containing  the  insoluble  matter  of  the  last  deter- 
mination at  a  low  red  heat,  cool,  and  weigh. 

SODIUM    CHLORID. 

Dissolve  3  to  5  grams  of  dye  in  200  cc  of  water,  acidify  the  solution 
with  nitric  acid,  and  precipitate  the  chloric  as  silver  chlorid.     The 

latter  is  separated,  unshed,  ignited,  and  weighed  in  a  tared  gooch 
crucible  in  the  usual  w  ay. 

SODIUM    SI  i  rn ate. 

Dissolve  i  gram  of  dye  in  about  100  cc  of  water  in  a  200-ce  gradu- 
ated flask,  add  10  cc  of  a  20  per  cent  solution  of  potassium  chlorid, 
shake,  the  mixture  well,  make  up  t<>  mark  with  water,  shake  agai^ 


212  COAL-TAR    COLORS   USED   IN    FOOD   PRODUCTS. 

and  then  filter  through  dry  paper.  Treat  100  cc  of  the  filtrate  (repre- 
senting 0.5  gram  of  dye)  with  5  cc  of  10  per  cent  barium  chlorid  solu- 
tion without  acidifying,  and  allow  to  stand  overnight.  If  a  precipi- 
tate forms,  it  is  filtered,  washed,  ignited,  and  weighed  in  the  usual 
way. 

HEAVY   METALS. 

Treat  the  sulphated  ash  from  1  gram  of  the  sample  with  20  cc  of 
water,  digest  with  10  cc  of  10  per  cent  hydrochloric  acid  till  solution 
is  complete,  place  3  cc  of  the  mixture  in  a  test  tube,  add  10  cc  of  freshly 
prepared  hydrogen  sulphid  test  solution  (U.  S.  P.),  shake  the  mixture, 
warm  to  50°  C,  stopper,  and  allow  to  stand  in  a  warm  place  (at  about 
35°  C.)  for  half  an  hour.  Run  a  blank  test  at  the  same  time,  with 
the  same  amount  of  hydrogen  sulphid  solution,  using  water  instead 
of  the  solution  containing  the  color  ash.  No  turbidity  other  than 
that  sometimes  produced  by  slight  separation  of  sulphur  should 
appear  in  this  test.  Both  tubes  are  then  made  slightly  alkaline 
with  ammonium  hydroxid,  and  no  precipitate  should  be  produced, 
although  a  slight  coloration,  due  to  the  presence  of  a  small  amount 
of  iron,  sometimes  occurs.  If  this  coloration  is  very  marked  the 
amount  of  iron  should  be  determined.  This  is  done  by  digesting  the 
sulphated  ash  from  a  weighed  amount  of  the  sample  with  hydrochloric 
acid  until  all  of  the  iron  has  gone  into  solution.  The  solution  is 
filtered,  and  the  filtrate  poured  into  an  excess  of  hot,  pure,  freshly 
prepared  sodium  hydroxid  (by  sodium)  solution  in  a  platinum  dish. 
The  precipitate  is  washed,  dissolved  in  dilute  hydrochloric  acid,  and 
again  precipitated  with  ammonium  hydroxid.  The  last  precipitate 
is  washed,  ignited,  and  weighed  in  the  usual  manner. 

ARSENIC    (SEEKER    AND    SMITIl's    METHOD). 

Dissolve  10  grams  of  the  dye  in  200  cc  of  water,  heating  to  insure 
complete  solution  of  the  color,  add  about  10  cc  of  strong  bromin  water 
to  convert  any  arsenite  to  arsenate.  Make  the  mixture  alkaline 
with  a  few  cubic  centimeters  of  strong  ammonium  hydroxid. 
Twenty  cubic  centimeters  of  a  sodium  phosphate  solution  containing 
100  grams  of  crystallized  sodium  phosphate  per  liter  are  next  added 
from  a  pipette,  after  which  magnesia  mixture  (containing  55  grams 
of  hydrated  magnesium  chlorid,  55  grams  of  ammonium  chlorid, 
and  88  CO  of  ammonium  hydroxid,  specific  gravity  0.9  per  liter)  is 
added  from  a  burette,  stirring  vigorously.  The  amount  of  mag- 
nesia added  should  be  in  slight  excess  of  that  necessary  completely  to 
precipitate  the  phosphate  and  should  previously  he  ascertained  hy 
blank  experiment.  Then  add  10  CC  of  ;inmionium  hydroxid  (specific 
gravity  0.90),  and  allow  the  whole  to  stand  for  at  least,  three  hours; 
separate  the  precipitate  hy  tiltration  and  wash  it  free,  or  nearly  so,  of 


METHODS   OF   ANALYSIS   FOR   CERTIFIED   COLORS. 


213 


,GLASS   ruB£  2.5 mnK 


dye  with  ammonium  hydroxid  containing  one-tenth  its  volume  of 
ammonia  (specific  gravity  0.90).  Dissolve  the  precipitate  from  the 
paper  with  1 : 1  nitric  acid,  the  washings  being  collected  in  a  large 
porcelain  crucible;  add  5  cc  of  sulphuric  acid  to  the  contents  of  the 
crucible,  and  evaporate  the  whole  almost  to  dryness.  It  is  not  nec- 
essary that  the  solution  should  be  colorless  at  this  point,  a  brown 
colored  solution  giving  equally  accurate  results.  Add  20  cc  of  water 
to  the  residue  in  the  crucible  and  then  10  cc  of 
a  saturated  solution  of  sulphur  dioxid;  evapo- 
rate the  solution  to  a  sirupy  consistency  to 
remove  the  sulphur  dioxid,  and  then  take  up 
in  20  cc  of  water  and  place  in  a  30-cc  evolution 
bottle,  add  5  cc  of  concentrated  sulphuric  acid, 
and  determine  the  arsenic  in  the  form  of  appa- 
ratus (fig.  1)  used  by  Bishop  in  his  modification 
of  the  Gutzeit  test,  the  stains  obtained  being 
compared  with  those  given  by  known  amounts 
of  arsenic. 

The  apparatus  used  by  Bishop  consists  of 
the  following  parts:  A  30-cc  salt  mouth  evo- 
lution bottle  into  which  is  fitted  a  one-hole 
rubber  stopper  carrying  a  glass  tube  6.5  cm 
long  with  an  internal  diameter  of  1  cm,  this 
tube  in  turn  being  provided  with  a  one-hole 
rubber  stopper  fitted  with  another  tube  of  the 
same  diameter  and  5.5  cm  long,  the  diameters 
of  both  tubes  being  constricted  at  the  points  at 
which  they  are  inserted  in  the  rubber  stoppers. 
A  third  glass  tube  15  cm  long,  having  an  in- 
ternal diameter  of  2.5  mm,  is  fitted  into  the 
second  at  its  upper  end  by  means  of  a  rubber 
stopper.  The  first  tube  contains  a  strip  of  filter 
paper  which  has  been  saturated  with  a  5  per 
cent  solution  of  lead  acetate  and  dried.  The 
second  tube  contains  a  loosely  packed  plug  of 
cotton-wool  freshly  moistened  with  a  1  percent  r„:.  i._Appmtaa  for  the 
solution  of  Lead  acetate.  Into  the  topmost  tube  aetanniMttaiofiiwoto. 
is  inserted  the  strip  of  sensitized  paper  to  receive  the  anenic  stain.  The 
arsin  is  generated  by  introducing  into  the  evolution  bottle  six  pieces  of 
Kahlbaum's  stick  zinc  (arsenic-free  for  forensic  purposes)  weighing 
in  all  about  s  grams,  and  t<>  assist  in  an  active  and  constant  evolution 

of  Lr;:s  a  disk  of  platinum  i-  also  [.laced  in  each  l>«>nl<>  to  form  an  elec- 
trolytic couple.      'I'll,-  evolution  of  gas  IS  allowed    to   proreed  for  one 

hour.    The  stains  are  produced  on  .strips  of  hard  pressed  w  hite  paper 
(2  nun  wide  and  120  mm  long)  that  has  been  sensitised  by  being 


H7TH  /%*>S.*C£T>4TT: 


^-SO/Pf  /crr» 


f>a.  *c£-n*nr  fww 


OZ  BOT-7ZS 


214         COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

dipped  in  a  5  per  cent  alcoholic  solution  of  mercuric  chlorid  and  then 
dried.  (Note. — It  has  recently  been  found  that  mere  uric  brornid  yields 
stains  that  are  more  evenly  distributed  and  also  produces  standards 
that  are  incomparably  more  permanent.)  For  purposes  of  com- 
parison it  is  better  not  to  develop  the  strips  stained  by  the  arsin, 
though  some  prefer  to  dip  the  stains  in  ammonium  hydroxid,  which 
causes  them  to  become  black.  A  blank  is  run  with  each  set  of 
determinations. 

ETHER    EXTRACTIVES. 

Dissolve  10  grams  of  color  in  150  cc  of  water  and  extract  in  a  separa- 
tory  funnel  with  ether  that  has  been  washed  with  water  (using  three 
150  cc  portions  of  water  for  each  liter  of  ether).  Extract  the  color 
solution  with  two  100  cc  portions  of  this  ether,  shaking  thoroughly 
for  one  minute,  and  wash  the  combined  ether  extract  successively 
with  35,  20,  and  10  cc  of  water  made  alkaline  or  acid,  as  the  case 
requires,  with  1  cc  of  tenth  normal  alkali  or  acid  per  100  cc  of  water. 
Decant  the  ether  from  the  mouth  of  the  separatory  and  rinse  the  funnel 
once  with  5  cc  ether.  The  color  solution  is  first  extracted  neutral, 
the  extracted  solution  being  then  rendered  alkaline  with  2  cc  of  a  10 
per  cent  solution  of  caustic  soda  and  again  extracted  with  two  100-cc 
portions  of  ether.  In  acidifying  for  the  third  extraction,  add  twice 
the  amount  of  hydrochloric  acid  (1  to  3)  necessary  to  neutralize  the 
alkali,  and  repeat  the  extraction  with  two  100-cc  portions  of  ether. 
Place  the  neutral,  alkaline,  and  acid  extracts  in  adust-free  atmosphere; 
and  allow  the  ether  to  evaporate  spontaneously,  after  which  dry  the 
residues  to  constant  weigh  over  sulphuric  acid,  using  flat-bottomed 
dishes  2 J  inches  in  diameter,  1}  inches  in  height,  and  of  about  100  cc 
capacity.  The  dishes  should  be  thoroughly  cleaned,  wiped  dry,  and 
allowed  to  stand  in  a  sulphuric  acid  desiccator  at  least  two  hours 
before  weighing.  In  order  to  avoid  the  generation  of  static  charges 
of  electricity,  they  should  not  be  wiped  immediately  before  weighing. 
Run  two  blank  determinations  with  each  series  of  ether  extracts,  and 
deduct  the  average  gain  in  weight  of  these  two  blanks  from  the  weights 
obtained  in  the  other  determinations. 

SULPIIATED    ASH. 

Weigh  accurately  0.5  to  1  gram  of  the  color  into  a  wide  platinum 
dish,  moisten  with  concentrated  sulphuric  acid,  and  ignite  cautiously, 
avoiding  spattering;  moisten  the  residue  repeatedly  with  sulphuric 
acid  and  ignite  until  all  the  carbon  is  removed  and  a  white  or  reddish 
ash  is  obtained.  This  is  finally  ignited  at  a  fairly  bright  red  heat, 
cooled,  and  weighed.  The  aqueous  solution  of  this  ash  should 
be  neutral  to  litmus,  and  may  bo  used  in  a  quantitative  test  for 
potassium. 


METHODS   OF   ANALYSIS   FOR  CERTIFIED  COLORS.  215 

CALCIUM. 

Digest  the  residue  from  the  sulphated  ash  determination  with 
hydrochloric  acid,  render  the  solution  alkaline  with  ammonium 
hydroxid,  filter,  and  precipitate  the  calcium  in  the  filtrate  with  ammo- 
nium oxalate.  The  precipitate  of  calcium  oxalate  is  filtered  on  a 
tared  gooch,  washed,  dried  at  100°  C.  and  weighed  as  calcium  oxalate, 
the  calcium  being  calculated  from  the  formula  CaC204.H20.  This 
method  is  applicable  only  in  cases  where  the  amount  of  calcium  is 
very  small.  When  the  amount  exceeds  0.5  per  cent  it  should  be 
determined  by  digesting  the  sulphated  ash  with  ammonium  sulphate 
solution  made  acid  with  hydrochloric  acid,  and  precipitating  the  iron 
by  an  excess  of  ammonium  hydroxid.  The  precipitate  is  washed, 
dissolved  in  hydrochloric  acid,  and  reprecipitated,  the  filtrate  and 
washings  being  added  to  those  obtained  from  the  first  precipitate. 
The  calcium  is  precipitated  in  the  combined  filtrates  with  ammonium 
oxalate,  the  oxalate  being  filtered,  washed,  ignited,  and  weighed  in 
the  usual  way;  the  residue  is  weighed  as  oxid  after  ignition  to  bright 
redness. 

SULPHUR. 

Determine  upon  0.2  to  0.3  gram  portions  by  the  Carius  method 
(Gattermann,  Practical  Methods  of  Organic  Chemistry,  1901,  p.  81), 
using  3  cc  of  fuming  nitric  acid  (sp.  gr.  1.5),  and  heating  the  sealed 
tubes  to  300°  C.  for  at  least  eight  hours. 

NITROGEN. 

Use  the  method  of  Dumas  (Gattermann,  Practical  Methods  of 
Organic  Chemistry,  1901,  p.  85). 

PONCEAU  3R. 

MOISTURE. 

Dry  1  to  2  grains  of  the  finely  ground  dye  at  109°  to  110°C.  in  a 
current  of  dry  hydrogen  to  constant  weight. 

TOTAL    INSOLUBLE    MATTER. 

Determine  as  under  Naphthol  Yellow  S,  page  211. 

\o\Yoi.ATILE    OR    INORGANIC    INSOLUBLE    MATTER. 

Determine  as  under  Naphthol  fellow  8,  i>.iLr«i  211. 

SODir.M   OHLOBID    (SESKEB    \\i>   KATHEWSOX'fl    Million). 

Mix  2  grama  of  dye  thoroughly  with  from  l}  to  3  grama  of  sodium 
carbonate,  moisten  with  water  to  form  a  paste,  again  mix.  dry,  and 
ignite  at  a  low  red  heat.     By  moistening,  drying,  and  reigniting  a 


216        COAL-TAR  COLORS  USED  IN  FOOD  PRODUCTS. 

more  complete  destruction  of  organic  matter  is  obtained.  Break  up 
the  charred  mass,  introduce  into  a  200-cc  graduated  flask  with  about 
100  to  150  cc  of  hot  water,  and  add  an  excess  of  potassium  perman- 
ganate to  oxidize  sulphids.  Destroy  the  excess  of  permanganate  by 
adding  sulphur  dioxid  solution  until  the  red  color  changes  to  brown, 
then  cool  the  mixture  and  make  up  to  the  mark  with  water.  Filter 
through  a  dry  paper,  acidify  100  cc  of  the  nitrate  with  nitric  acid, 
and  precipitate  the  chlorin  as  silver  chlorid  by  the  addition  of  silver 
nitrate.  If  the  solution  should  be  brownish  from  a  trace  of  organic 
matter  the  silver  chlorid  does  not  readily  coagulate  and  tends  to  pass 
through  the  filter.  In  this  case  a  few  drops  of  potassium  permanganate 
solution  are  added  to  this  acid  mixture,  the  organic  matter  being 
almost  instantly  oxidized.  The  mixture  is  then  decolorized  with  a 
few  drops  of  sulphur  dioxid  solution,  the  silver  chlorid  is  separated  on 
a  tared  gooch,  washed,  ignited,  and  weighed  in  the  usual  manner. 
The  following  method  may  also  be  used  for  Ponceau  3R: 
Dissolve  5  grams  of  the  dye  in  15C  cc  hot  water,  wash  into  a  250-cc 
graduated  flask,  and  add  25  cc  of  a  10  per  cent  solution  of  barium 
nitrate.  Cool  the  mixture,  make  up  to  the  mark,  and  filter  through  a 
dry  paper;  acidify  100  cc  of  the  nitrate,  representing  2  grains  of  color, 
with  nitric  acid,  and  treat  with  silver  nitrate  solution,  the  precipi- 
tated silver  chlorid  being  separated,  washed,  ignited,  and  weighed  in  a 
tared  gooch  crucible  in  the  usual  way. 

SODIUM    SULPHATE. 

Dissolve  2  grams  of  dye  in  100  cc  of  hot  water,  wash  into  a  200-cc 
graduated  flask,  add  50  grams  of  pure  sodium  chlorid,  cool,  and  make 
up  to  the  mark  with  water.  Filter  through  a  dry  filter,  dilute  100  cc 
of  the  filtrate  to  300  cc,  acidify  with  hydrochloric  acid  and  precipi- 
tate the  sulphates  with  barium  chlorid.  Filter,  wash,  ignite,  and 
weigh  in  a  tared  platinum  gooch  in  the  usual  way. 

HEAVY   METALS. 

Determine  as  given  under  Naphthol  Yellow  S,  page  212. 

ARSENIC. 

Determine  as  given  under  Naphthol  Yellow  S,  page  212. 

ETHER    EXTRACTIVES. 

Determine  OS  given  under  Naphthol  Yellow  S,  page  214. 

SULPHATED    ASH. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214. 


METHODS   OF   ANALYSIS   FOR    CERTIFIED    COLORS.  217 

CALCIUM. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215. 

SULPHUR. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215. 

NITROGEN    (SEEKER   AND   MATHEWSOX's    METHOD). 

Treat  2  grams  of  the  color  with  25  cc  of  a  saturated  solution  of 
sulphur  dioxid  and  1  gram  of  zinc  dust  and  warm  the  mixture  gently 
until  it  becomes  colorless.  This  should  take  place  in  from  two  to  three 
minutes,  but  if  it  does  not  add  more  sulphur  dioxid  solution  in  small 
portions  at  a  time  until  the  color  is  destroyed.  Then  add  30  cc  of  con- 
centrated sulphuric  acid  and  0.7  gram  of  mercuric  oxid  or  its  equiva- 
lent of  metallic  mercury  and  digest  the  mixture,  make  alkaline,  and 
distil  as  directed  on  page  6,  Bulletin  107,  Revised,  Bureau  of  Chemistry, 
United  States  Department  of  Agriculture,  under  the  Kjeldahl  process. 

CRUDE    CUMIDIN. 

Dissolve  20  grams  of  dye  in  400  cc  of  hot  water  and  pour  the  solu- 
tion, a  little  at  a  time,  into  a  reducing  solution  composed  of  75  grams 
of  stannous  chlorid  dissolved  in  180  cc  of  concentrated  hydrochloric 
acid.  Heat  the  mixture  on  a  steam  bath  until  it  is  straw  colored, 
cool,  add  an  excess  of  sodium  hydroxid,  and  extract  in  a  separatory 
runnel  with  ether.  Separate  the  ether  layer  and  distil  off  the  solvent 
until  the  residue  measures  about  50  cc.  Then  cautiously  heat  over 
the  steam  with  constant  agitation  until  the  odor  of  ether  disappears, 
after  which  the  last  of  the  moisture  is  removed  by  introducing  a  few 
pieces  of  solid  caustic  soda  and  allowing  to  stand.  The  residue  con- 
sists of  crude  cumidin  and  should  boil  above  220°  C.  Cumidin 
nitrate  is  sparingly  soluble  in  water. 

ORANGE  I. 

MOISTURE. 

Determine  as  given  under  Ponceau  3K,  page  215. 

TOTAL    INSOLUBLE    MATTER 

Determine  ;>^  given  under  Naphthol  Yellow  8,  page  211. 

NONVOL  \  I  ill.   OB    INORGANIC    EN80LUBLI    maitku. 

Determine  ;i-  given  under  Naphthol  Yellow  s.  page  211, 

SODD  m    (  BLOBJB. 

Determine  afl  given  under  Ponceau  3R,  page  215. 


218  COAL-TAR   COLORS   USED   IN    FOOD   PRODUCTS. 

SODIUM    SULPHATE. 

Dissolve  1  gram  of  dye  in  100  cc  water  contained  m  a  200-cc  grad- 
uated flask  and  treat  the  solution  with  60  cc  of  a  20  per  cent  solution 
of  potassium  chlorid.  Make  the  mixture  up  to  the  mark  with 
water,  shake,  filter  through  a  diy  paper,  dilute  an  aliquot  of  100  cc 
of  the  filtrate  to  200  cc,  acidify  with  1  cc  of  10  per  cent  hydro- 
chloric acid,  treat  with  5  cc  of  10  per  cent  barium  chlorid  solution, 
and  allow  to  stand  over  night.  If  a  precipitate  has  been  formed 
this  is  separated,  ignited,  and  weighed  in  the  usual  way. 

HEAVY    METALS. 

Determine  as  given  under  Xaphthol  Yellow  S,  page  212. 

ARSENIC    (SEEKER   AND    SMITH' S    METHOD). 

Dissolve  2  grams  of  dye  in  a  mixture  of  130  cc  water  and  70  cc  of 
95  per  cent  alcohol.  Add  about  10  cc  of  strong  bromin  water  to 
convert  any  arsenite  to  arsenate.  Make  the  mixture  alkaline  with  a 
few  cubic  centimeters  of  strong  ammonium  hydroxid  and  add,  from 
a  pipette,  20  cc  of  a  sodium  phosphate  solution  containing  100 
grams  of  crystallized  sodium  phosphate  per  liter,  after  which  mag- 
nesia mixture  (containing  55  grams  of  hydrated  magnesium  chlorid, 
55  grams  of  ammonium  chlorid,  and  88  cc  of  ammonium  hydroxid, 
sp.  gr.  0.9,  per  liter)  is  added  from  a  burette,  stirring  vigorously. 
The  amount  of  magnesia  mixture  to  be  added  should  be  in  slight 
excess  of  that  necessary  to  precipitate  the  phosphate  completely, 
and  should  be  previously  ascertained  by  a  blank  experiment.  Finally 
add  10  cc  of  ammonium  hydroxid  (sp.  gr.  0.96)  and  allow  the  whole 
to  stand  for  at  least  eight  hours.  Separate  the  precipitate  by  filtra- 
tion and  wash  it  free,  or  nearly  so,  of  dye  with  a  mixture  of  one-third 
alcohol  and  two-thirds  water  containing  one-tenth  its  volume  of 
ammonium  hydroxid  (sp.  gr.  0.90) .  Dissolve  the  precipitate  from  the 
paper  with  20  per  cent  sulphuric  acid,  the  washings  being  collected 
in  a  large  porcelain  crucible.  Add  5  cc  of  concentrated  nitric  acid 
to  the  contents  of  the  crucible  and  evaporate  the  whole  almost  to 
dryness.  The  mixture  need  not  be  colorless  at  this  point,  a  brown 
colored  solution  giving  equally  accurate  results.  Add  20  cc  of  water 
to  the  residue  in  the  crucible  and  then  10  cc  of  a  saturated  solution 
of  sulphur  dioxid.  Evaporate  the  solution  to  a  syrupy  consistency 
to  remove  sulphur  dioxid,  and  then  take  up  in  20  cc  of  water,  place 
in  a  30-cc  evolution  bottle,  add  5  cc  of  concentrated  sulphuric  acid, 
and  determine  the  arsenic  by  the  modified  Gutzeit  method  as  given 
under  Naphthol  Yellow  8,  page  213. 

BTHEB    EXTRACTIVES. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214 


METHODS    OF   ANALYSIS   FOR    CERTIFIED    COLORS.  219 

SULPHATED    ASH. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214. 

CALCIUM. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215. 

SULPHUR. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215. 

NITROGEN. 

Determine  as  given  under  Ponceau  3R,  page  217. 

TEST   FOR   ORANGE    II    (SMITH   AND   MATHEWSON's   METHOD). 

The  following  solutions  are  required : 

(1)  Fifteen  per  cent  titanium  trichlorid. 

(2)  Freshly  prepared  diazotized  sulphanilic  acid.  Heat  a  mixture 
composed  of  1  gram  of  sulphanilic  acid,  10  cc  of  water,  and  20  cc  of 
concentrated  hydrochloric  acid  on  a  steam  bath  for  five  minutes  with 
occasional  shaking.  Cool  to  about  10°  C.  and  add  slowly  10  cc  of  a  1 
per  cent  solution  of  sodium  nitrite.  Allow  the  mixture  to  stand  at 
about  10°  for  10  minutes,  dilute  to  1  liter,  and  shake  until  all  the 
solid  particles  have  dissolved. 

(3)  Stannous  chlorid,  prepared  by  dissolving  40  grams  of  stannous 
chlorid  in  100  cc  of  concentrated  hydrochloric  acid.  Dilute  this  ten 
times  with  water,  immediately  before  using. 

Place  2  cc  of  a  0.1  per  cent  solution  of  the  dye  in  a  colorimeter  tube 
having  a  capacity  of  about  100  cc,  add  a  small  drop  of  titanium  trichlo- 
rid solution  and  shake  until  the  mixture  is  decolorized.  Standards 
containing  the  same  quantity  of  color  composed  of  a  mixture  of  pure 
Orange  I  and  known  amounts  of  Orange  II  are  treated  in  the  same 
way,  the  volume  of  the  solution  at  this  point  to  measure  less  than  5  cc. 
Dilute  the  decolorized  solutions  to  50  cc  with  95  per  cent  alcohol  and 
equalize  the  temperature4  by  immersing  the  tubes  in  water  at  room 
temperature.  (Note. — A  slight  coloration  that  may  develop  at  this 
point  may  bo  disregarded.)  Allow  the  tubes  to  stand  in  the  water 
for  about  five  minute-,  add  2  cc  of  the  diazotized  sulphanilic  acid, 
and  mix  thoroughly.  If  the  titanium  trichlorid  has  not  been  used 
in  too  great  excess,  the  first  few  drops  of  the  diazotized  sulphanilic 
acid  will  cause  a  formation  of  color.  Allow  the  coupling  to  proceed 
for  three  minutes  and  then  add  5  CC  of  the  diluted  BtannOUS  chlorid 

with  vigorous  shaking.     In  two  minutes  the  blue  color  due  t«»  (  tarange  I 
will  disappear j  Leaving  only  (he  pink  caused  by  the  coupling  product 

of  Orange  II.    The  depth  of  color  in  the  tube  containing  the  dye 
under  examination  may  then  he  compared  to  the  standards. 


220  COAL-TAR   COLORS  USED   EN   FOOD  PRODUCTS. 

AMARANTH. 
MOISTURE. 

Determine  as  given  under  Ponceau  3R,  page  215. 

TOTAL    INSOLUBLE    MATTER. 

Determine  as  given  under  Naphthol  Yellow  S,  page  211. 

NONVOLATILE    OR    INORGANIC    INSOLUBLE    MATTER. 

Determine  as  given  under  Naphthol  Yellow  S,  page  211. 

SODIUM    CHLORID. 

Determine  as  given  under  Ponceau  3R,  page  215. 

SODIUM    SULPHATE. 

Dissolve  2  grams  of  dye  in  100  cc  of  warm  water  in  a  200-cc  grad- 
uated flask,  and  add  36  grams  of  pure  sodium  chlorid.  Allow  the 
mixture  to  stand  with  frequent  shaking  for  one  hour,  and  after  cooling 
make  up  to  the  mark  with  a  saturated  salt  solution.  Shake  the 
mixture  and  fdter  through  a  dry  paper;  dilute  100  cc  of  the  filtrate 
(representing  1  gram)  with  water,  acidify  with  hydrochloric  acid,  and 
precipitate  the  sulphates  with  barium  chlorid.  The  precipitate  is 
separated,  washed,  and  ignited  upon  a  tared  platinum  gooch  crucible. 

HEAVY   METALS. 

Determine  as  given  under  Naphthol  Yellow  S,  page  212. 

ARSENIC. 

Determine  as  given  under  Naphthol  Yellow  S,  page  212. 

ETHER    EXTRACTIVES. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214. 

SULPHATED   ASH. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214. 

CALCIUM. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215. 

SULPHUR. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215. 


METHODS   OF  ANALYSIS   FOR   CERTIFIED  COLORS.  221 

NITROGEN. 

Determine  as  given  under  Ponceau  3R,  page  217. 

LIGHT  GREEN  S  F  YELLOWISH. 
MOISTURE. 

Determine  as  given  under  Ponceau  3R,  page  215. 

TOTAL    INSOLUBLE    MATTER. 

Determine  as  given  under  Naphthol  Yellow  S,  page  211. 

NONVOLATILE    OR    INORGANIC    INSOLUBLE    MATTER. 

Determine  as  given  under  Xaphthol  Yellow  S,  page  211. 

SODIUM    CULORID. 

Determine  as  given  under  Ponceau  3R,  page  215. 

SODIUM    SULPHATE. 

Dissolve  5  grams  of  the  color  in  100  cc  of  water,  warming  by  means 
of  a  gentle  heat.  Dissolve  1 1  grams  of  safranin  in  a  separate  portion 
of  400  cc  of  water,  also  by  warming,  taking  care  in  both  instances  to 
prevent  loss  by  evaporation.  Mix  the  two  solutions,  shake  thor- 
oughly, and  niter  through  a  diy  filter.  Render  an  aliquot  portion 
of  the  filtrate  alkaline  with  sodium  hydroxid  and  remove  the  excess 
of  safranin  by  shaking  with  two  successive  portions  of  amyl  alcohol. 
Wash  the  combined  amyl  alcohol  layers  with  two  portions  of  water 
and  add  the  washings  to  the  main  aqueous  solution,  which  is  then 
acidified  with  hydrochloiic  acid  and  sulphates  determined  in  the  usual 
manner  by  preciptiation  with  barium  chlorid  as  barium  sulphate. 

JILAYY    METALS. 

Determine  as  given  under  Xaphthol  Yellow  S,  page  212. 

ARSENIC. 

Determine  as  given  under  Naphthol  Yellow  S,  page  212. 
1:1  mi:    EXTRACTIVES. 

Determine  as  given  under  Naphthol  Yellow  S,  page  21  I 

Si  i  I'll  \  I  I  i)   ASH. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214. 

1  (II    M. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215 


222        COAlrTAR  COLORS  USED  IN  FOOD  PRODUCTS. 

SULPHUR. 

Determine  as  given  under  Naphthol  Yellow  S,  page  215. 

NITROGEN. 

Determine  on  2-gram  portions  by  Gunning's  modification  of  the 
Kjeldahl  process,  using  a  little  copper  sulphate  to  assist  the  oxidation 
(see  page  7,  Bulletin  107,  Revised,  Bureau  of  Chemistry,  United 
States  Department  of  Agriculture). 

ERYTHROSIN. 
MOISTURE. 

Determine  as  given  under  Ponceau  3R,  page  215. 

TOTAL    INSOLUBLE    MATTER. 

Determine  as  given  under  Naphthol  Yellow  S,  page  211. 

NONVOLATILE    OR    INORGANIC    INSOLUBLE   MATTER 

Determine  as  given  under  Naphthol  Yellow  S,  page  211. 

SODIUM    CHLORID. 

Dissolve  5  grams  of  the  dye  in  400  cc  water  and  acidify  with  dilute 
nitric  acid.  Make  the  mixture  up  to  500  cc  with  water,  and  then 
filter  through  a  dry  filter.  Determine  chlorids  in  an  aliquot  of  200  cc 
of  the  filtrate  by  precipitation  with  silver  nitrate,  washing,  igniting, 
and  weighing  the  silver  chlorid  in  a  tared  gooch  crucible  in  the  usual 
manner. 

SODIUM    SULPHATE. 

Employ  another  aliquot  of  the  filtrate  obtained  after  precipitating 
the  color  acid  as  above  in  the  determination  of  sulphates,  precipi- 
tating the  latter  as  barium  sulphate  in  the  usual  manner. 

HEAVY   METALS. 

Determine  as  given  under  Naphthol  Yellow  S,  page  212. 

ARSENIC    (SEEKER   AND    SMITH'S    METHOD). 

Dissolve  16  grams  of  dye  in  370  cc  of  water,  add  5  cc  of  strong 
bromin  water,  and  finally  25  cc  of  dilute  sulphuric  acid  (1  to  4). 
Shake  thoroughly  and  filter  through  a  dry  filter.  Place  an  aliquot 
of  250  cc,  representing  10  grams  of  color  from  the  filtrate,  in  a  porce- 
lain casserole,  add  5  cc  concentrated  nitric  acid  (very  important  to 
prevent  loss  of  arsenic),  and  evaporate  till  fuming  has  ceased.  Reduce 
the  residue  with  sulphur  dioxid  solution,  evaporate  to  small  hulk, 
and  determine  the  arsenic  in  the  form  of  apparatus  used  by  Bishop  in 


METHODS   OF   ANALYSIS   FOR    CERTIFIED   COLORS.  223 

his  modification  of  the  Gutzeit  test.  See  under  Naphthol  Yellow  S, 
pages  212  and  213.  (Note.— It  is  somewhat  difficult  at  times  to 
recover  250  cc  of  filtrate,  but  less  may  be  used  and  a  correction  made, 
if  necessary.) 

ETHER    EXTRACTIVES. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214,  omitting 
the  acid  extraction. 

SULPHATED    ASH. 

Determine  as  given  under  Naphthol  Yellow  S,  page  214. 

IODIN,  BROMIN,  AND    CHLORIN    (CORNELISON'S    METHOD). 

Mix  0.2  to  0.3  gram  of  the  sample  with  2  grams  of  pure  potassium 
bichromate  and  15  cc  of  strong  sulphuric  acid  in  the  evolution  flask 
of  an  apparatus  made  entirely  of  glass,  with  ground-glass  joints. 
Thoroughly  mix  the  contents  of  the  evolution  flask,  so  that  all  lumps 
are  disintegrated,  and  then  heat  at  100°  C.  for  15  minutes,  after 
which  raise  the  temperature  to  150°  C.  for  thirty  minutes,  a  cur- 
rent of  air  dried  over  calcium  chlorid  and  potassium  hydroxid  being 
drawn  through  the  apparatus  during  this  time.  Iodin  remains  in 
the  evolution  flask  as  iodic  acid;  bromin  passes  off  as  such,  and  may 
be  absorbed  by  allowing  the  air  passing  through  the  apparatus  to 
bubble  through  1  per  cent  sodium  hydroxid.  Chlorin  passes  out  of 
the  evolution  flask  as  chromyl  chlorid,  and  may  also  be  absorbed  in 
sodium  hydroxid.  Cool  the  mixture  containing  the  iodic  acid,  and 
reduce  the  chromic  acid  by  addition  of  sulphur  dioxid,  about  20  cc 
of  a  saturated  solution  being  required.  When  enough  has  been 
added,  the  precipitated  iodin  redissolves,  and  the  clear  green  color 
of  chrome  alum  appears.  Filter,  wash  the  paper  with  distilled  water, 
dilute  the  filtrate  and  washings  to  about  300  cc,  and  add  an  excess  of 
silver  nitrate.  Boil  till  the  silver  iodid  has  flocculated,  allow  to  stand 
for  a  few  hours,  and  separate  and  weigh  the  silver  iodid  in  a  tared 
gooch. 

It  sometimes  happens  that  the  mixture  containing  the  iodic  acid, 
after  the  reduction  with  sulphur  dioxid,  becomes  turbid,  owing, 
apparently,  to  separation  of  a  basic  chromium  Bulphate.  Very  often 
the  turbidity  can  not  be  removed  by  filtering,  and  it  lias  been  found 
advisable  in  this  case  to  reject  the  determination  and  begin  anew. 


IODIN    (SEEKKK    AM)    MATHEWSON'S    METHOD).1 

Place  from  0.3  to  0.4  gram  of  the  crythrosin  in  a  porcelain  casserol, 
dissolve  this  in  5  cc  of  a  10  per  cent  Bodium  hydroxid  solution,  then 
add  :;.">  <•<•  of  a  7  per  cent  solution  of  potassium  permanganate.     After 

lU.  8.  .  BnraM  "f  Chflmlstry  'reulur  (>o.     The  tttlmattftll  uf  iodin  in  organic  coiiijhhiiwLs 

an<l  ii     wptnttion  from  othflt  ball 


224         COAL-TAR  COLORS  USED  IN  POOD  PRODUCTS. 

mixing,  cover  the  vessel  with  a  watch  crystal,  and  add  10  cc  of 
nitric  acid,  keeping  the  dish  covered.  Agitate  the  mixture,  place 
on  a  steam  bath,  and  keep  covered  until  spattering  ceases,  after 
which  remove  the  watch  glass  and  allow  evaporation  to  proceed  to 
dryness.1  Treat  the  residue  with  5  cc  of  7  per  cent  potassium  per- 
manganate and  5  cc  of  concentrated  nitric  acid  and  again  evaporate 
to  dryness.  Then  add  about  50  cc  of  water  and  5  cc  of  concentrated 
nitric  acid  to  the  residue,  following  this  by  40  cc  of  a  saturated  solu- 
tion of  sulphur  dioxid,  and  allow  the  whole  to  stand  with  occasional 
stirring  (breaking  up  the  lumps  with  a  glass  rod)  until  the  hydrated 
oxid  of  manganese  has  dissolved.  Filter,  and  wash  the  paper  with 
water.  Add  an  excess  of  silver  nitrate  to  the  nitrate,  and  boil  until 
sulphur  dioxid  has  been  expelled  and  the  silver  iodid  has  flocculated. 
Separate,  wash,  and  weigh  the  precipitate  in  the  usual  manner. 

TOTAL    HALOGENS. 

Mix  0.5  to  1  gram  of  the  dye  with  4  grams  of  potassium  carbonate, 
moisten  to  a  paste,  again  thoroughly  mix,  cover  with  a  layer  of  dry 
potassium  carbonate,  dry,  and  ignite  at  a  low  red  heat.  Break  up 
the  char  thoroughly,  digest  with  about  200  cc  water,  and  filter. 
Wash  the  insoluble  matter  until  the  washings  no  longer  react  with 
silver  nitrate;  then  acidify  the  filter  and  washings  with  nitric  acid 
and  precipitate  the  halogens  in  the  usual  way  as  silver  salts. 

INDIGO  DISULPHOACID. 
MOISTURE. 

Determine  as  given  under  Ponceau  3R,  page  215. 

TOTAL    INSOLUBLE    MATTER. 

Determine  as  given  under  Naphthol  Yellow  S,  page  211. 

NONVOLATILE    OR    INORGANIC    INSOLUBLE    MATTER. 

Determine  as  given  under  Naphthol  Yellow  S,  page  211. 

SODIUM    CHLORID. 

Determine  as  given  under  Ponceau  3R,  page  215. 

SODIUM    SULPHATE. 

Dissolve  2  grams  of  the  dye  in  about  L60  cc  <>f  water  and  treat  the 

solutioo  wit  1 1   lo  giams  <>!'  pure  Bodium  chlorid.     Aftei  the  salt  has 

olved,  make  up  the  volume  to  exactly  200  cc.    Shake  the  mix- 

•  in  1 1  !<■  operation  of  drying  particular  can  should  be  obaerved  to  prevent  aoce  a  of  reducing  gases  to  the 
mixture. 


ADDENDA.  225 

ture  thoroughly  and  filter  through  a  dry  filter.  Dilute  50  cc  of  the 
filtrate  with  200  cc  of  water,  acidify  with  1  cc  of  10  per  cent  hydro- 
chloric acid,  and  treat  with  an  excess  of  barium  chlorid  solution. 
After  standing  overnight,  the  precipitate  is  separated,  washed, 
ignited,  and  weighed  in  the  usual  way. 

HEAVY    METALS. 

Determine  as  given  under  Xaphthol  Yellow  S,  page  212. 

ARSENIC    (SEEKER    AND    SMITH ; 8    METHOD). 

Treat  10  grams  of  dye  in  a  Kjeldahl  flask  with  100  cc  water  and 
10  cc  concentrated  nitric  acid.  Warm  gently  and  finally  boil  until 
all  action  has  ceased.  Transfer  to  a  beaker,  make  alkaline  with 
ammonium  hydroxid,  and  proceed  from  this  point,  as  in  the  case  of 
the  solution  of  Xaphthol  Yellow  S,  page  212,  continuing  from  the 
point  at  which  sodium  phosphate  is  added. 

ETHER    EXTRACTIVES. 

Dissolve  3  grams  of  dye  in  200  cc  of  water  and  extract  with  ether. 
as  directed  under  Xaphthol  Yellow  S.  page  214. 

8ULPHATED    ASH. 

Determine  as  given  under  Xaphthol  Yellow  S.  page  214. 

CALCIUM. 

Determine  as  given  under  Xaphthol  Yellow  S.  page  215. 

SULPHUR. 

Determine  a-  given  under  Xaphthol  Yellow  S.  page  215. 

NITROGEN. 

Determine  as  given  under  Light  Green  SF  Yellowish,  page  222. 

XVIII.  ADDENDA. 

ADDITIONAL  EXAMINATION  OF  COAL-TAR  DYES. 

Since  the  foregoing  report  was  written  the  chemical  examination  of 
the  coal-tar  dye  specimens  collected  in  the  summer  of  1907  has  been 
completed.  This  investigaf  ion  shows  that  7  of  the  ( rreen  Table  num- 
bers then  reported  were  not,  mi  i  he  market .  although  those  funushing 
the  specimens  included  them  at,  the  time  that  the  samples  were  sup- 
plied.    These  numbers  are  as  follow-:  not  physiologically  examined, 

<!       Hull.  L47-  12 15 


226  COAL-TAR    COLORS    USED   IN    FOOD   PRODUCTS. 

G.  T.  49,  60,  104,  5 IS,  523;  physiologically  examined,  with  unfavora- 
ble result,  G.  T.  516;  with  favorable  result,  G.  T.  520. 

The  chemical  examination  also  shows  that  each  of  9  additional 
Green  Table  numbers  occurred  once  among  the  unreported  numbers. 
They  are  as  follows:  not  examined  physiologically,  G.  T.  20,  328; 
examined  physiologically:  with  unfavorable  results,  G.  T.  602;  with 
favorable  results,  G.  T.  92,  477,  521 ;  with  contradictory  results,  G.  T. 
16,  43,  163.  G.  T.  20  is  anilin  azo  (1:8)  dioxy  naphthalene  (3:6) 
disulpho  acid.  G.  T.  -J28  is  diamino-stilbene-disulpho  acid-disazo- 
phenol. 

This  chemical  examination  finally  shows  that  beside  the  Green 
Table  numbers  there  occurred,  once  each,  the  following:  sulphonated 
Victoria  Blue  B  and  a  sulphonated  rjiodulin  and  twice,  amido-azo- 
toluene-azo-alpha-naphthol. 

It  is  clear  that  this  revised  statement  of  facts  is  without  influence 
on  the  7  permitted  dyes  selected;  its  only  effect  is  to  add  G.  T.  92 
(yellow),  477  (blue),  and  521  (red)  (each  occurring  but  once)  to,  and 
to  subtract  520  (red)  (said  to  occur  twice)  from,  the  16  dyes  (page  166) 
from  among  which  the  7  permitted  dyes  were  selected,  thus  giving  18 
instead  of  16  dyes  to  choose  from;  however,  the  final  selection  is 
wholly  unaffected  thereby.  It  is  also  clear  that  any  and  all  inter- 
mediate conclusions  or  comparisons  are  only  slightly  and  immaterially 
affected,  if  at  all,  by  the  results  of  this  additional  examination. 


SUPPLEMENTARY  LIST  OF  TRADE  NAMES  OF  COAL-TAR  COLORS. 


Arid  Yellow  S  (4). 

Alkali  Blue  (47 

Azo  Acid  Rubin  2B  (107). 

Azo  Yellow  (92). 

Crocein  Scarlet  0  extra  (104). 

Dimethylanilin  Orange  (87). 

Eosin,  water  soluble  (512). 

Fast  Red  A  (102). 

Fast  Red  B  (65). 

Fast  Red  E  (105;. 

Fast  Yellow  Y  (8). 

Indian  Yellow  (92). 


Indulin  R  and  B  (601] . 

Leucindophenol  (572 

Methyl  Orange    - 

Naphthylamin  Pink 

Naphthylene  Blue  R  in  crystals  (639). 

SolubleBlue  8B  and  10B  (479). 

Sulphur  Yellow  (4). 

Thiochromogen  (659). 

Victoria  Blue  (488). 

Wool  Black  (166). 

Yellow  T 


XIX.  INDEX  OF  AUTHORITIES  QUOTED. 


[References  arc  made  to  important  citations  exclusive  of  pages  76  to  LS2,  except  in  cases  where  the  author 

is  notcitfi  elsewhere.] 


Page. 

Arloing  and  ( !azeneuve 90 

Beckh 55 

B6hal 177 

Bergeron  and  Clouct 1 19 

Beythien  and  Hempel 17;] 

Bishop 213 

rny 54 

Braune                               121 

Buss 71 

Cazeneuve 93 

Leave  and  Arloing 

"live  and  Lepine 

Chlopin 59,72, 

Clouet  and  BergeroD L19 

Combemale  and  Francos L42 

Confed  ione  

Dietrich 

Krdmann 44,57 

170 

akel,  .1 25 

Fraenkel,  8... 

ttd  ( tombemale L42 


Prentzel . . . . 
Galliard  .  .  . 

•  ■  and  Braunschweig 


121 


( rreen,  Arthur  G 

Gudeman 

Beidenhain 

iel  &  Beythien 

Henley 

If-  ughtoo 

Huoppe 

mational    White    Croes    Con- 



Kayeer 

Koberi 

Koenig 

Kohnstamm,  E.  <  ■ 

Lehmann 

Lupine  A  I  aaei  euve. 
Lewio ... 

Lieber 

Ludwig 

Meyer 

Mmtcl.M 

National    <  Son  i 

Lion  



Patent-.  11    R.  O  mmittet    >n... 
. 

etto 


L5 
24 

52 

17:; 
25 

34 

171' 
44 

3 

190 

.7.  L57 

12 

B 

74 

i,  191 

24,  eo 

171 


1 1 
id 


228 


OAL-TAR  COLORS  USED  IX  FOOD  PRODUCTS. 


lJa^ 


Rose:.- 


54     v.  Raumer. 


Santori 47, 158 

Schacher: 45,  75, 191 

Schultz 56 

Society  of  Swiss  Analytical  (hem- 

ifitfl 43,  75 

Stilling 55,  56,  57, 180 

Canton  of  Tessin 75 

Tschirch 43,  57 


Page. 

37 

Weyl 23,  24,  26,  4  i,  58, 181 

Weyl  (Leffman  translation) 14, 

37,  74, 179, 181 

^ft'illiams,  H.  W 55 

Winogradow 52 

Winton 24, 59 

Young 1 50 


O 


) 


ss>' 


lliliiiii 

3  1262  09216  9118 


